Quantum computers based on electron spins controlled by ultrafast off-resonant single optical pulses.

PubMed

Clark, Susan M; Fu, Kai-Mei C; Ladd, Thaddeus D; Yamamoto, Yoshihisa

2007-07-27

We describe a fast quantum computer based on optically controlled electron spins in charged quantum dots that are coupled to microcavities. This scheme uses broadband optical pulses to rotate electron spins and provide the clock signal to the system. Nonlocal two-qubit gates are performed by phase shifts induced by electron spins on laser pulses propagating along a shared waveguide. Numerical simulations of this scheme demonstrate high-fidelity single-qubit and two-qubit gates with operation times comparable to the inverse Zeeman frequency.

The indispensable role of the transversal spin fluctuations mechanism in laser-induced demagnetization of Co/Pt multilayers with nanoscale magnetic domains.

PubMed

Zhang, Wei; He, Wei; Peng, Li-Cong; Zhang, Ying; Cai, Jian-Wang; Evans, Richard F L; Zhang, Xiang-Qun; Cheng, Zhao-Hua

2018-07-06

The switching of magnetic domains induced by an ultrashort laser pulse has been demonstrated in nanostructured ferromagnetic films. This leads to the dawn of a new era in breaking the ultimate physical limit for the speed of magnetic switching and manipulation, which is relevant to current and future information storage. However, our understanding of the interactions between light and spins in magnetic heterostructures with nanoscale domain structures is still lacking. Here, both time-resolved magneto-optical Kerr effect experiments and atomistic simulations are carried out to investigate the dominant mechanism of laser-induced ultrafast demagnetization in [Co/Pt] 20 multilayers with nanoscale magnetic domains. It is found that the ultrafast demagnetization time remains constant with various magnetic configurations, indicating that the domain structures play a minor role in laser-induced ultrafast demagnetization. In addition, both in experiment and atomistic simulations, we find a dependence of ultrafast demagnetization time τ M on the laser fluence, which is in contrast to the observations of spin transport within magnetic domains. The remarkable agreement between experiment and atomistic simulations indicates that the local dissipation of spin angular momentum is the dominant demagnetization mechanism in this system. More interestingly, we made a comparison between the atomistic spin dynamic simulation and the longitudinal spin flip model, highlighting that the transversal spin fluctuations mechanism is responsible for the ultrafast demagnetization in the case of inhomogeneous magnetic structures. This is a significant advance in clarifying the microscopic mechanism underlying the process of ultrafast demagnetization in inhomogeneous magnetic structures.

Tunable room-temperature spin-selective optical Stark effect in solution-processed layered halide perovskites

PubMed Central

Giovanni, David; Chong, Wee Kiang; Dewi, Herlina Arianita; Thirumal, Krishnamoorthy; Neogi, Ishita; Ramesh, Ramamoorthy; Mhaisalkar, Subodh; Mathews, Nripan; Sum, Tze Chien

2016-01-01

Ultrafast spin manipulation for opto–spin logic applications requires material systems that have strong spin-selective light-matter interaction. Conventional inorganic semiconductor nanostructures [for example, epitaxial II to VI quantum dots and III to V multiple quantum wells (MQWs)] are considered forerunners but encounter challenges such as lattice matching and cryogenic cooling requirements. Two-dimensional halide perovskite semiconductors, combining intrinsic tunable MQW structures and large oscillator strengths with facile solution processability, can offer breakthroughs in this area. We demonstrate novel room-temperature, strong ultrafast spin-selective optical Stark effect in solution-processed (C6H4FC2H4NH3)2PbI4 perovskite thin films. Exciton spin states are selectively tuned by ~6.3 meV using circularly polarized optical pulses without any external photonic cavity (that is, corresponding to a Rabi energy of ~55 meV and equivalent to applying a 70 T magnetic field), which is much larger than any conventional system. The facile halide and organic replacement in these perovskites affords control of the dielectric confinement and thus presents a straightforward strategy for tuning light-matter coupling strength. PMID:27386583

Nonthermal ultrafast optical control of the magnetization in garnet films

NASA Astrophysics Data System (ADS)

Hansteen, Fredrik; Kimel, Alexey; Kirilyuk, Andrei; Rasing, Theo

2006-01-01

We demonstrate coherent optical control of the magnetization in ferrimagnetic garnet films on the femtosecond time scale through a combination of two different ultrafast and nonthermal photomagnetic effects and by employing multiple pump pulses. Linearly polarized laser pulses are shown to create a long-lived modification of the magnetocrystalline anisotropy via optically induced electron transfer between nonequivalent ion sites while circularly polarized pulses additionally act as strong transient magnetic field pulses originating from the nonabsorptive inverse Faraday effect. Due to the slow phonon-magnon interaction in these dielectrics, thermal effects of the laser excitation are clearly distinguished from the ultrafast nonthermal effects and can be seen only on the time scale of nanoseconds for sample temperatures near the Curie point. The reported effects open exciting possibilities for ultrafast manipulation of spins by light, and provide insight into the physics of magnetism on ultrafast time scales.

Design and commissioning of an aberration-corrected ultrafast spin-polarized low energy electron microscope with multiple electron sources.

PubMed

Wan, Weishi; Yu, Lei; Zhu, Lin; Yang, Xiaodong; Wei, Zheng; Liu, Jefferson Zhe; Feng, Jun; Kunze, Kai; Schaff, Oliver; Tromp, Ruud; Tang, Wen-Xin

2017-03-01

We describe the design and commissioning of a novel aberration-corrected low energy electron microscope (AC-LEEM). A third magnetic prism array (MPA) is added to the standard AC-LEEM with two prism arrays, allowing the incorporation of an ultrafast spin-polarized electron source alongside the standard cold field emission electron source, without degrading spatial resolution. The high degree of symmetries of the AC-LEEM are utilized while we design the electron optics of the ultrafast spin-polarized electron source, so as to minimize the deleterious effect of time broadening, while maintaining full control of electron spin. A spatial resolution of 2nm and temporal resolution of 10ps (ps) are expected in the future time resolved aberration-corrected spin-polarized LEEM (TR-AC-SPLEEM). The commissioning of the three-prism AC-LEEM has been successfully finished with the cold field emission source, with a spatial resolution below 2nm. Copyright © 2017 Elsevier B.V. All rights reserved.

Perspective: Ultrafast magnetism and THz spintronics

NASA Astrophysics Data System (ADS)

Walowski, Jakob; Münzenberg, Markus

2016-10-01

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

Control of Terahertz Emission by Ultrafast Spin-Charge Current Conversion at Rashba Interfaces

NASA Astrophysics Data System (ADS)

Jungfleisch, Matthias B.; Zhang, Qi; Zhang, Wei; Pearson, John E.; Schaller, Richard D.; Wen, Haidan; Hoffmann, Axel

2018-05-01

We show that a femtosecond spin-current pulse can generate terahertz (THz) transients at Rashba interfaces between two nonmagnetic materials. Our results unambiguously demonstrate the importance of the interface in this conversion process that we interpret in terms of the inverse Rashba Edelstein effect, in contrast to the THz emission in the bulk conversion process via the inverse spin-Hall effect. Furthermore, we show that at Rashba interfaces the THz-field amplitude can be controlled by the helicity of the light. The optical generation of electric photocurrents by these interfacial effects in the femtosecond regime will open up new opportunities in ultrafast spintronics.

Control of Terahertz Emission by Ultrafast Spin-Charge Current Conversion at Rashba Interfaces.

PubMed

Jungfleisch, Matthias B; Zhang, Qi; Zhang, Wei; Pearson, John E; Schaller, Richard D; Wen, Haidan; Hoffmann, Axel

2018-05-18

We show that a femtosecond spin-current pulse can generate terahertz (THz) transients at Rashba interfaces between two nonmagnetic materials. Our results unambiguously demonstrate the importance of the interface in this conversion process that we interpret in terms of the inverse Rashba Edelstein effect, in contrast to the THz emission in the bulk conversion process via the inverse spin-Hall effect. Furthermore, we show that at Rashba interfaces the THz-field amplitude can be controlled by the helicity of the light. The optical generation of electric photocurrents by these interfacial effects in the femtosecond regime will open up new opportunities in ultrafast spintronics.

Perspective: Ultrafast magnetism and THz spintronics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Walowski, Jakob; Münzenberg, Markus

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledgemore » the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.« less

Ultrafast intersystem-crossing in platinum containing π-conjugated polymers with tunable spin-orbit coupling.

PubMed

Sheng, C-X; Singh, S; Gambetta, A; Drori, T; Tong, M; Tretiak, S; Vardeny, Z V

2013-01-01

The development of efficient organic light-emitting diodes (OLED) and organic photovoltaic cells requires control over the dynamics of spin sensitive excitations. Embedding heavy metal atoms in π-conjugated polymer chains enhances the spin-orbit coupling (SOC), and thus facilitates intersystem crossing (ISC) from the singlet to triplet manifolds. Here we use various nonlinear optical spectroscopies such as two-photon absorption and electroabsorption in conjunction with electronic structure calculations, for studying the energies, emission bands and ultrafast dynamics of spin photoexcitations in two newly synthesized π-conjugated polymers that contain intrachain platinum (Pt) atoms separated by one (Pt-1) or three (Pt-3) organic spacer units. The controllable SOC in these polymers leads to a record ISC time of <~1 ps in Pt-1 and ~6 ps in Pt-3. The tunable ultrafast ISC rate modulates the intensity ratio of the phosphorescence and fluorescence emission bands, with potential applications for white OLEDs.

Complex Terahertz and Direct Current Inverse Spin Hall Effect in YIG/Cu1-xIrx Bilayers Across a Wide Concentration Range.

PubMed

Cramer, Joel; Seifert, Tom; Kronenberg, Alexander; Fuhrmann, Felix; Jakob, Gerhard; Jourdan, Martin; Kampfrath, Tobias; Kläui, Mathias

2018-02-14

We measure the inverse spin Hall effect of Cu 1-x Ir x thin films on yttrium iron garnet over a wide range of Ir concentrations (0.05 ⩽ x ⩽ 0.7). Spin currents are triggered through the spin Seebeck effect, either by a continuous (dc) temperature gradient or by ultrafast optical heating of the metal layer. The spin Hall current is detected by electrical contacts or measurement of the emitted terahertz radiation. With both approaches, we reveal the same Ir concentration dependence that follows a novel complex, nonmonotonous behavior as compared to previous studies. For small Ir concentrations a signal minimum is observed, whereas a pronounced maximum appears near the equiatomic composition. We identify this behavior as originating from the interplay of different spin Hall mechanisms as well as a concentration-dependent variation of the integrated spin current density in Cu 1-x Ir x . The coinciding results obtained for dc and ultrafast stimuli provide further support that the spin Seebeck effect extends to terahertz frequencies, thus enabling a transfer of established spintronic measurement schemes into the terahertz regime. Our findings also show that the studied material allows for efficient spin-to-charge conversion even on ultrafast time scales.

Non-thermal optical excitation of terahertz-spin precession in a magneto-optical insulator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parchenko, Sergii; Maziewski, Andrzej; Stupakiewicz, Andrzej, E-mail: and@uwb.edu.pl

2016-01-18

We demonstrate non-thermal ultrafast laser excitation of spin precession with THz frequency in Gd-Bi-substituted iron garnet via the inverse Faraday effect. The modulation of THz precession by about 60 GHz below the compensation temperature of magnetic moment was observed. The THz frequency precession was caused by the exchange resonance between the Gd and Fe sublattices; we attributed the low-frequency modulation to dielectric resonance mode with a magnetic contribution. We demonstrate the possibility of polarization-sensitive control of spin precession under THz generation by laser pulses, helping to develop high-speed magneto-optical devices.

Momentum space view of the ultrafast dynamics of surface photocurrents on topological insulators

NASA Astrophysics Data System (ADS)

Kuroda, K.; Reimann, J.; Güdde, J.; Höfer, U.

2017-02-01

The Dirac-cone surface states of topological insulators are characterized by a chiral spin texture in k-space with the electron spin locked to its parallel momentum. Mid-infrared pump pulses can induce spin-polarized photocurrents in such a topological surface state by optical transitions between the occupied and unoccupied part of the Dirac cone. We monitor the ultrafast dynamics of the corresponding asymmetric electron population in momentum space directly by time- and angle-resolved two-photon photoemission (2PPE). The elastic scattering times of 2.5 ps deduced for Sb2Te3 corresponds to a mean-fee path of 0.75 μm in real space.

Using ultrashort terahertz pulses to directly probe spin dynamics in insulating antiferromagnets

NASA Astrophysics Data System (ADS)

Bowlan, P.; Trugman, S. A.; Yarotski, D. A.; Taylor, A. J.; Prasankumar, R. P.

2018-05-01

Terahertz pulses are a direct and general probe of ultrafast spin dynamics in insulating antiferromagnets (AFM). This is shown by using optical-pump, THz-probe spectroscopy to directly track AFM spin dynamics in the hexagonal multiferroic HoMnO3 and the orthorhombic multiferroic TbMnO3. Our studies show that despite the different structural and spin orders in these materials, THz pulses can unambiguously resolve spin dynamics after optical photoexcitation. We believe that this approach is quite general and can be applied to a broad range of materials with different AFM spin alignments, providing a novel non-contact approach for probing AFM order with femtosecond temporal resolution.

Lattice-mediated magnetic order melting in TbMnO 3

DOE PAGES

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.; ...

2018-03-15

Recent ultrafast magnetic-sensitive measurements have revealed a delayed melting of the long-range cycloid spin order in TbMnO 3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting andmore » is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. In conclusion, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.« less

Lattice-mediated magnetic order melting in TbMnO 3

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.

Recent ultrafast magnetic-sensitive measurements have revealed a delayed melting of the long-range cycloid spin order in TbMnO 3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting andmore » is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. In conclusion, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.« less

All-optical spin switching: A new frontier in femtomagnetism — A short review and a simple theory

NASA Astrophysics Data System (ADS)

Zhang, G. P.; Latta, T.; Babyak, Z.; Bai, Y. H.; George, Thomas F.

2016-08-01

Using an ultrafast laser pulse to manipulate the spin degree of freedom has broad technological appeal. It allows one to control the spin dynamics on a femtosecond time scale. The discipline, commonly called femtomagnetism, started with the pioneering experiment by Beaurepaire and coworkers in 1996, who showed subpicosecond demagnetization occurs in magnetic Ni thin films. This finding has motivated extensive research worldwide. All-optical helicity-dependent spin switching (AO-HDS) represents a new frontier in femtomagnetism, where a single ultrafast laser pulse can permanently switch spin without any assistance from a magnetic field. This review summarizes some of the crucial aspects of this new discipline: key experimental findings, leading mechanisms, controversial issues, and possible future directions. The emphasis is on our latest investigation. We first develop the all-optical spin switching (AOS) rule that determines how the switchability depends on the light helicity. This rule allows one to understand microscopically how the spin is reversed and why the circularly polarized light appears more powerful than the linearly polarized light. Then we invoke our latest spin-orbit coupled harmonic oscillator model to simulate single spin reversal. We consider both continuous wave (cw) excitation and pulsed laser excitation. The results are in a good agreement with the experimental result (a MatLab code is available upon request from the author). We then extend the code to include the exchange interaction among different spin sites. We show where the “inverse-Faraday field” comes from and how the laser affects the spin reversal nonlinearly. Our hope is that this review will motivate new experimental and theoretical investigations and discussions.

Quantum Entanglement of Quantum Dot Spin Using Flying Qubits

DTIC Science & Technology

2015-05-01

QUANTUM ENTANGLEMENT OF QUANTUM DOT SPIN USING FLYING QUBITS UNIVERSITY OF MICHIGAN MAY 2015 FINAL TECHNICAL REPORT APPROVED FOR PUBLIC RELEASE...To) SEP 2012 – DEC 2014 4. TITLE AND SUBTITLE QUANTUM ENTANGLEMENT OF QUANTUM DOT SPIN USING FLYING QUBITS 5a. CONTRACT NUMBER FA8750-12-2-0333...been to advance the frontier of quantum entangled semiconductor electrons using ultrafast optical techniques. The approach is based on

Unifying ultrafast demagnetization and intrinsic Gilbert damping in Co/Ni bilayers with electronic relaxation near the Fermi surface

NASA Astrophysics Data System (ADS)

Zhang, Wei; He, Wei; Zhang, Xiang-Qun; Cheng, Zhao-Hua; Teng, Jiao; Fähnle, Manfred

2017-12-01

The ability to controllably manipulate the laser-induced ultrafast magnetic dynamics is a prerequisite for future high-speed spintronic devices. The optimization of devices requires the controllability of the ultrafast demagnetization time τM and intrinsic Gilbert damping αintr. In previous attempts to establish a relationship between τM and αintr, the rare-earth doping of a permalloy film with two different demagnetization mechanisms was not a suitable candidate. Here, we choose Co/Ni bilayers to investigate the relations between τM and αintr by means of the time-resolved magneto-optical Kerr effect (TR-MOKE) via adjusting the thickness of the Ni layers, and obtain an approximately proportional relation between these two parameters. The remarkable agreement between the TR-MOKE experiment and the prediction of a breathing Fermi-surface model confirms that a large Elliott-Yafet spin-mixing parameter b2 is relevant to the strong spin-orbital coupling at the Co/Ni interface. More importantly, a proportional relation between τM and αintr in such metallic films or heterostructures with electronic relaxation near the Fermi surface suggests the local spin-flip scattering dominates the mechanism of ultrafast demagnetization, otherwise the spin-current mechanism dominates. It is an effective method to distinguish the dominant contributions to ultrafast magnetic quenching in metallic heterostructures by simultaneously investigating both the ultrafast demagnetization time and Gilbert damping. Our work can open an avenue to manipulate the magnitude and efficiency of terahertz emission in metallic heterostructures such as perpendicular magnetic anisotropic Ta/Pt/Co/Ni/Pt/Ta multilayers, and then it has an immediate implication for the design of high-frequency spintronic devices.

Surface Plasmon-Mediated Nanoscale Localization of Laser-Driven sub-Terahertz Spin Dynamics in Magnetic Dielectrics

NASA Astrophysics Data System (ADS)

Chekhov, Alexander L.; Stognij, Alexander I.; Satoh, Takuya; Murzina, Tatiana V.; Razdolski, Ilya; Stupakiewicz, Andrzej

2018-05-01

Ultrafast all-optical control of spins with femtosecond laser pulses is one of the hot topics at the crossroads of photonics and magnetism with a direct impact on future magnetic recording. Unveiling light-assisted recording mechanisms for an increase of the bit density beyond the diffraction limit without excessive heating of the recording medium is an open challenge. Here we show that surface plasmon-polaritons in hybrid metal-dielectric structures can provide spatial confinement of the inverse Faraday effect, mediating the excitation of localized coherent spin precession with 0.41 THz frequency. We demonstrate a two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within the 100 nm layer in dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways towards non-thermal opto-magnetic recording at the nano-scale.

EDITORIAL: Ultrafast magnetization processes

NASA Astrophysics Data System (ADS)

Hillebrands, Burkard

2008-09-01

This Cluster Issue of Journal of Physics D: Applied Physics is devoted to ultrafast magnetization processes. It reports on the scientific yield of the Priority Programme 1133 'Ultrafast Magnetization Processes' which was funded by the Deutsche Forschungsgemeinschaft in the period 2002-2008 in three successive two-year funding periods, supporting research of 17-18 groups in Germany. Now, at the end of this Priority Programme, the members feel that the achievements made in the course of the programme merit communication to the international scientific community in a concerted way. Therefore, each of the projects of the last funding period presents a key result in a published contribution to this Cluster Issue. The purpose of the funding by a Priority Programme is to advance knowledge in an emerging field of research through collaborative networked support over several locations. Priority Programmes are characterized by their enhanced quality of research through the use of new methods and forms of collaboration in emerging fields, by added value through interdisciplinary cooperation, and by networking. The aim of the Priority Programme 1133 'Ultrafast Magnetization Processes' may be well characterized by the call for projects in June 2001 after the programme was approved by the Deutsche Forschungsgemeinschaft: 'The aim of the priority programme is the achievement of a basic understanding of the temporal evolution of fast magnetization processes in magnetically ordered films, multilayers and micro-structured systems. The challenge lies in the advancement of the field of ultrafast magnetization processes into the regime of a few femtoseconds to nanoseconds, a topic not yet well explored. A general aim is to understand the fundamental mechanisms needed for applications in ultrafast magneto-electronic devices. The fundamental topic to be addressed is the response of the magnetization of small structures upon the application of pulsed magnetic fields, laser pulses or injected spin-polarized electron pulses on short time scales, ranging from a small disturbance of the system up to the reversal of the magnetization direction.' Now, seven years later, the subject of ultrafast magnetization processes has grown into a mainstream research direction in modern magnetism. The major international conferences on magnetism, such as the Annual Conference on Magnetism and Magnetic Materials (MMM), the INTERMAG, the International Conference of Magnetism, as well as many regional conferences, schedule dedicated sessions to ultrafast magnetization processes, very often several of them. The large share in research in this field from German scientists has been made possible by this Priority Programme. Since its beginning, new developments have been picked up by the Priority Programme 1133 and addressed by projects. Spin torque phenomena in spin dynamics, although foreseen at the time of establishing the Priority Programme, have been taken up. The field of dissipation has been addressed and extended by several groups, with contributions both from theoretical and experimental groups. A first set of contributions addresses ultrafast dynamics and materials. T Roth et al [article 164001] in this issue] study the dynamics of coercivity in ultrafast pump-probe experiments on the femtosecond time scale. They show that an all optical pump-probe technique is, in general, not suitable for gaining access to the time-dependent behaviour of the coercivity, since the switching in a fixed external field is an irreversible process. They comment on the possible mechanisms leading to the observed reduction of the coercivity with increasing pump power and propose a potential solution to clarify the origin of such a behaviour. B Heitkamp et al [164002] discuss the femtosecond spin dynamics of ferromagnetic CoPt thin films and nanodots, which they probe using spin-polarized photoemission electron microscopy. They show by photoelectron spin analysis, that enhanced optical near fields can be used to induce a local demagnetization of the sample following femtosecond laser excitation. A B Schmidt et al [164003] report a new access to the surface electronic structure of fcc Co films combining spin-resolved one- and two-photon photoemission. The knowledge of surface states is important for interpreting time-resolved measurements of ultrafast magnetization dynamics in this material. An extension of ultrafast dynamics has been made by several groups. A Melnikov et al [164004] report on the ultrafast dynamics at lanthanide surfaces such as Gd(0001) and Tb(0001) using time-resolved second-harmonic generation and photoelectron spectroscopy. These surfaces exhibit a rich dynamics including a collective response of the crystal lattice and the magnetization. Effects of phonon-magnon scattering are discussed. M Fiebig et al [164005] report on experiments of ultrafast magnetization dynamics in antiferromagnetic compounds, and show that the magnetization dynamics in these systems differs noticeably from that of ferromagnetic compounds. They use optical second-harmonic generation and linear reflection to monitor the evolution of the antiferromagnetic order parameter subsequent to an intense optical excitation. In a theory paper, the local light-induced spin manipulation in two-magnetic-centre metallic chains is studied by T Hardenstein et al [164006] using highly correlational ab initio calculations. They show that, as an example of local spin manipulation, the spin on the iron side of a Co-Na-Fe cluster can be switched. S Halm et al [164007] present evidence to manipulate spin states in a diluted magnetic semiconductor on a submicrometer length scale via the magnetic fringe fields of micro-structured magnets. By optically switching the magnetization of the ferromagnet, the magnetization in the semiconductor is manipulated and the limits of a dynamical interaction between the spin states in the ferromagnet and the magnetic semiconductor are discussed. A second set of contributions addresses the field of spin waves and dynamic spin torque phenomena. C W Sandweg et al [164008] discuss the modification of the thermal spin wave spectrum by a domain wall in a narrow stripe and report the observation of a localized mode near the domain wall using the new technique of Brillouin light scattering microscopy. Time-resolved measurements are often made using a stroboscopic approach, thus missing non-periodic responses. P Möhrke et al [164009] report single-shot Kerr magnetometer measurements to observe the real time-domain wall motion in permalloy nanowires. The dynamics in magnetic disks is studied by I Neudecker et al [164010] using in-plane magnetic microwave fields for excitation. The effect of current-induced magnetization dynamics in single and double layer magnetic nanopillars is reported by N Müsgens et al [164011]. A spin-polarized charge current can modify the damping properties of spin waves in magnetic nanostructures. This is reported by V E Demidov et al [164012] using space-resolved Brillouin light scattering. They also present results regarding nonlinear spin-wave propagation and mode coupling in magnetic stripes and squares. D V Berkov and N L Gorn [164013] report on their results of nonlinear magnetization dynamics in nanodevices induced by a spin-polarized current using micromagnetic simulation. A third set of contributions focuses on dissipation phenomena ranging from a phenomenological description to the investigation of the microscopic origin(s). In a theory paper, M Fähnle et al [164014] revisit the Gilbert equation and discuss anisotropic and non-local damping of the magnetization dynamics. They derive their results by a combination of the breathing Fermi surface model with a variant of the ab initio density functional electron theory given by the magnetic force theorem. On the experimental side, S Serrano-Guisan et al [164015] address Gilbert damping in Ni81Fe19 thin films and microstructures using anisotropic magnetoresistance and pulsed inductive microwave magnetometry to measure the time-resolved precessional magnetization dynamics. The intrinsic and non-local Gilbert damping in polycrystalline Ni films is also addressed by J Walowski et al [164016] using femtosecond laser pulses. Several spin-wave modes are observed and their dissipation is studied. Non-local damping by spin currents emitted into a non-magnetic metallic layer of either vanadium, palladium or dysprosium is studied. Dissipation in small magnetic Ni81Fe19 rings is studied using Brillouin light scattering microscopy by H Schultheiss et al [164017]. They investigate the spatial profiles and the decay constants of spin-wave quasi-eigenmodes. We hope that this cluster of papers will help to stimulate and advance a better understanding of this very interesting field of ultrafast magnetization processes.

Field-controlled ultrafast magnetization dynamics in two-dimensional nanoscale ferromagnetic antidot arrays

PubMed Central

De, Anulekha; Mondal, Sucheta; Sahoo, Sourav; Barman, Saswati; Otani, Yoshichika; Mitra, Rajib Kumar

2018-01-01

Ferromagnetic antidot arrays have emerged as a system of tremendous interest due to their interesting spin configuration and dynamics as well as their potential applications in magnetic storage, memory, logic, communications and sensing devices. Here, we report experimental and numerical investigation of ultrafast magnetization dynamics in a new type of antidot lattice in the form of triangular-shaped Ni80Fe20 antidots arranged in a hexagonal array. Time-resolved magneto-optical Kerr effect and micromagnetic simulations have been exploited to study the magnetization precession and spin-wave modes of the antidot lattice with varying lattice constant and in-plane orientation of the bias-magnetic field. A remarkable variation in the spin-wave modes with the orientation of in-plane bias magnetic field is found to be associated with the conversion of extended spin-wave modes to quantized ones and vice versa. The lattice constant also influences this variation in spin-wave spectra and spin-wave mode profiles. These observations are important for potential applications of the antidot lattices with triangular holes in future magnonic and spintronic devices. PMID:29719763

Ultrafast Magnetization of a Dense Molecular Gas with an Optical Centrifuge.

PubMed

Milner, A A; Korobenko, A; Milner, V

2017-06-16

Strong laser-induced magnetization of oxygen gas at room temperature and atmospheric pressure is achieved experimentally on the subnanosecond time scale. The method is based on controlling the electronic spin of paramagnetic molecules by means of manipulating their rotation with an optical centrifuge. Spin-rotational coupling results in a high degree of spin polarization on the order of one Bohr magneton per centrifuged molecule. Owing to the nonresonant interaction with the laser pulses, the demonstrated technique is applicable to a broad class of paramagnetic rotors. Executed in a high-density gas, it may offer an efficient way of generating macroscopic magnetic fields remotely (as shown in this work) and producing a large amount of spin-polarized electrons.

Ultrafast Magnetization of a Dense Molecular Gas with an Optical Centrifuge

NASA Astrophysics Data System (ADS)

Milner, A. A.; Korobenko, A.; Milner, V.

2017-06-01

Strong laser-induced magnetization of oxygen gas at room temperature and atmospheric pressure is achieved experimentally on the subnanosecond time scale. The method is based on controlling the electronic spin of paramagnetic molecules by means of manipulating their rotation with an optical centrifuge. Spin-rotational coupling results in a high degree of spin polarization on the order of one Bohr magneton per centrifuged molecule. Owing to the nonresonant interaction with the laser pulses, the demonstrated technique is applicable to a broad class of paramagnetic rotors. Executed in a high-density gas, it may offer an efficient way of generating macroscopic magnetic fields remotely (as shown in this work) and producing a large amount of spin-polarized electrons.

Is perpendicular magnetic anisotropy essential to all-optical ultrafast spin reversal in ferromagnets?

NASA Astrophysics Data System (ADS)

Zhang, G. P.; Bai, Y. H.; George, Thomas F.

2017-10-01

All-optical spin reversal presents a new opportunity for spin manipulations, free of a magnetic field. Most of all-optical-spin-reversal ferromagnets are found to have a perpendicular magnetic anisotropy (PMA), but it has been unknown whether PMA is necessary for spin reversal. Here we theoretically investigate magnetic thin films with either PMA or in-plane magnetic anisotropy (IMA). Our results show that spin reversal in IMA systems is possible, but only with a longer laser pulse and within a narrow laser parameter region. Spin reversal does not show a strong helicity dependence where the left- and right-circularly polarized light lead to the identical results. By contrast, the spin reversal in PMA systems is robust, provided both the spin angular momentum and laser field are strong enough while the magnetic anisotropy itself is not too strong. This explains why experimentally the majority of all-optical spin-reversal samples are found to have strong PMA and why spins in Fe nanoparticles only cant out of plane. It is the laser-induced spin-orbit torque that plays a key role in the spin reversal. Surprisingly, the same spin-orbit torque results in laser-induced spin rectification in spin-mixed configuration, a prediction that can be tested experimentally. Our results clearly point out that PMA is essential to spin reversal, though there is an opportunity for in-plane spin reversal.

Observation of sub-100-fs optical response from spin-coated films of squarylium dye J aggregates

NASA Astrophysics Data System (ADS)

Furuki, Makoto; Tian, Minquan; Sato, Yasuhiro; Pu, Lyong Sun; Kawashima, Hitoshi; Tatsuura, Satoshi; Wada, Osamu

2001-04-01

For spin-coated films of squarylium dye J aggregates, ultrafast nonlinear optical responses were investigated by pump-probe measurements. By using a broadband mode-locked titanium:sapphire laser, we succeeded in observing the optical response with a time resolution of better than 60 fs. Time-resolved transmission data are shown for different excitation wavelengths, resonant to the excitonic absorption band and off-resonant. Relaxation times of the absorption saturation were evaluated to be 140 fs (fast component) and 950 fs (slow component) in the case of resonant excitation and 98 fs in the case of off-resonant excitation.

Homepage P. Fischer, LBNL, Berkeley CA | UC Santa Cruz CA

Science.gov Websites

mesoscale magnetic x-ray microscopy and spectroscopy (ultra-)fast spin dynamics soft x-ray tomography of condensed matter x-ray optics publications presentations invited talks conference contributions curriculum

Lattice-mediated magnetic order melting in TbMnO3

NASA Astrophysics Data System (ADS)

Baldini, Edoardo; Kubacka, Teresa; Mallett, Benjamin P. P.; Ma, Chao; Koohpayeh, Seyed M.; Zhu, Yimei; Bernhard, Christian; Johnson, Steven L.; Carbone, Fabrizio

2018-03-01

Recent ultrafast magnetic-sensitive measurements [Johnson et al., Phys. Rev. B 92, 184429 (2015), 10.1103/PhysRevB.92.184429; Bothschafter et al., Phys. Rev. B 96, 184414 (2017), 10.1103/PhysRevB.96.184414] have revealed a delayed melting of the long-range cycloid spin order in TbMnO3 following photoexcitation across the fundamental Mott-Hubbard gap. The microscopic mechanism behind this slow transfer of energy from the photoexcited carriers to the spin degrees of freedom is still elusive and not understood. Here, we address this problem by combining spectroscopic ellipsometry, ultrafast broadband optical spectroscopy, and ab initio calculations. Upon photoexcitation, we observe the emergence of a complex collective response, which is due to high-energy coherent optical phonons coupled to the out-of-equilibrium charge density. This response precedes the magnetic order melting and is interpreted as the fingerprint of the formation of anti-Jahn-Teller polarons. We propose that the charge localization in a long-lived self-trapped state hinders the emission of magnons and other spin-flip mechanisms, causing the energy transfer from the charge to the spin system to be mediated by the reorganization of the lattice. Furthermore, we provide evidence for the coherent excitation of a phonon mode associated with the ferroelectric phase transition.

Measurements of ultrafast spin-profiles and spin-diffusion properties in the domain wall area at a metal/ferromagnetic film interface.

PubMed

Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Manfredda, M; Kiskinova, M; Zabel, H; Kläui, M; Lüning, J; Pietsch, U; Gutt, C

2017-11-08

Exciting a ferromagnetic material with an ultrashort IR laser pulse is known to induce spin dynamics by heating the spin system and by ultrafast spin diffusion processes. Here, we report on measurements of spin-profiles and spin diffusion properties in the vicinity of domain walls in the interface region between a metallic Al layer and a ferromagnetic Co/Pd thin film upon IR excitation. We followed the ultrafast temporal evolution by means of an ultrafast resonant magnetic scattering experiment in surface scattering geometry, which enables us to exploit the evolution of the domain network within a 1/e distance of 3 nm to 5 nm from the Al/FM film interface. We observe a magnetization-reversal close to the domain wall boundaries that becomes more pronounced closer to the Al/FM film interface. This magnetization-reversal is driven by the different transport properties of majority and minority carriers through a magnetically disordered domain network. Its finite lateral extension has allowed us to measure the ultrafast spin-diffusion coefficients and ultrafast spin velocities for majority and minority carriers upon IR excitation.

Spin-coated Films of Squarylium Dye J-Aggregates Exhibiting Ultrafast Optical Responses

NASA Astrophysics Data System (ADS)

Tatsuura, Satoshi; Tian, Minquan; Furuki, Makoto; Sato, Yasuhiro; Pu, Lyong Sun; Wada, Osamu

2000-08-01

The formation of J-aggregates of squarylium dye derivatives in spin-coated films is reported. Squarylium dye derivatives with dipropylamino bases are found to spontaneously aggregate in a spin-coated film. Aggregation is promoted when dye molecules are dispersed in a poly(vinyl alcohol) film, and when a spin-coated film of dye molecules is heated in the presence of acid vapor. In particular, J-aggregates formed by exposure to acetic acid vapor show the narrowest spectral width. J-aggregates formed by the acid treatment method are stable at room temperature and the spectral full-width at half maximum of the J-band is 20 nm. Optical response of the acid-treated film is confirmed to exhibit a short relaxation time of bleached absorption of 300 fs.

Ultrafast Photoinduced Multimode Antiferromagnetic Spin Dynamics in Exchange-Coupled Fe/RFeO3 (R = Er or Dy) Heterostructures.

PubMed

Tang, Jin; Ke, Yajiao; He, Wei; Zhang, Xiangqun; Zhang, Wei; Li, Na; Zhang, Yongsheng; Li, Yan; Cheng, Zhaohua

2018-05-25

Antiferromagnetic spin dynamics is important for both fundamental and applied antiferromagnetic spintronic devices; however, it is rarely explored by external fields because of the strong exchange interaction in antiferromagnetic materials. Here, the photoinduced excitation of ultrafast antiferromagnetic spin dynamics is achieved by capping antiferromagnetic RFeO 3 (R = Er or Dy) with an exchange-coupled ferromagnetic Fe film. Compared with antiferromagnetic spin dynamics of bare RFeO 3 orthoferrite single crystals, which can be triggered effectively by ultrafast laser heating just below the phase transition temperature, the ultrafast photoinduced multimode antiferromagnetic spin dynamic modes, for exchange-coupled Fe/RFeO 3 heterostructures, including quasiferromagnetic resonance, impurity, coherent phonon, and quasiantiferromagnetic modes, are observed in a temperature range of 10-300 K. These experimental results not only offer an effective means to trigger ultrafast antiferromagnetic spin dynamics of rare-earth orthoferrites, but also shed light on the ultrafast manipulation of antiferromagnetic magnetization in Fe/RFeO 3 heterostructures. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Excitation and doping dependence of hole-spin relaxation in bulk GaAs

NASA Astrophysics Data System (ADS)

Krauss, Michael; Hilton, David; Schneider, Hans Christian

2009-03-01

We present theoretical and experimental results on ultrafast hole-spin dynamics in bulk GaAs. By combining a sufficiently realistic bandstructure at the level of an 8x8 k .p theory and a dynamical treatment of the relevant scattering mechanisms [1], we obtain quantitative agreement between the microscopic theoretical results and differential transmission measurements [2] for different excitation conditions. In particular, we examine the dependence of the hole-spin relaxation time on the optically excited carrier density, lattice temperature, and doping concentration. Although the spin relaxation is rather insensitive to changes in the optically excited density and temperature, strong p-doping causes a significantly faster relaxation. [1] M. Krauss, M. Aeschlimann, and H. C. Schneider, Phys.Rev.Lett. 100, 256601 (2008)[2] D. J. Hilton and C. L. Tang, Phys. Rev. Lett. 89, 146601 (2002)

Ultrafast Manipulation of Magnetic Order with Electrical Pulses

NASA Astrophysics Data System (ADS)

Yang, Yang

During the last 30 years spintronics has been a very rapidly expanding field leading to lots of new interesting physics and applications. As with most technology-oriented fields, spintronics strives to control devices with very low energy consumption and high speed. The combination of spin and electronics inherent to spintronics directly tackles energy efficiency, due to the non-volatility of magnetism. However, speed of operation of spintronic devices is still rather limited ( nanoseconds), due to slow magnetization precessional frequencies. Ultrafast magnetism (or opto-magnetism) is a relatively new field that has been very active in the last 20 years. The main idea is that intense femtosecond laser pulses can be used in order to manipulate the magnetization at very fast time-scales ( 100 femtoseconds). However, the use of femtosecond lasers poses great application challenges such as diffraction limited optical spot sizes which hinders device density, and bulky and expensive integration of femtosecond lasers into devices. In this thesis, our efforts to combine ultrafast magnetism and spintronics are presented. First, we show that the magnetization of ferrimagnetic GdFeCo films can be switched by picosecond electronic heat current pulses. This result shows that a non-thermal distribution of electrons directly excited by laser is not necessary for inducing ultrafast magnetic dynamics. Then, we fabricate photoconductive switch devices on a LT-GaAs substrate, to generate picosecond electrical pulses. Intense electrical pulses with 10ps (FWHM) duration and peak current up to 3A can be generated and delivered into magnetic films. Distinct magnetic dynamics in CoPt films are found between direct optical heating and electrical heating. More importantly, by delivering picosecond electrical pulses into GdFeCo films, we are able to deterministically reverse the magnetization of GdFeCo within 10ps. This is more than one order of magnitude faster than any other electrically controlled magnetic switching. Our results present a fundamentally new switching mechanism electrically, without requirement for any spin polarized current or spin transfer/orbit torques. Our discovery that ultrafast magnetization switching can be achieved with electrical pulses will launch a new frontier of spintronics science and herald a new generation of spintronic devices that operate at high speed with low energy consumption. At last, to push ultrafast spintronics to practical use, ultrafast switching of a ferromagnetic film is desired. By exploiting the exchange interaction between GdFeCo and ferromagnetic Co/Pt layer, we achieved ultrafast (sub 10ps) switching of ferromagnetic film with a single laser pulse. This result will open up the possibility to control ferromagnetic materials at ultrafast time scale, critical for practical applications.

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE PAGES

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai; ...

2017-10-23

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Henn, T.; Kiessling, T., E-mail: tobias.kiessling@physik.uni-wuerzburg.de; Ossau, W.

We describe a two-color pump-probe scanning magneto-optical Kerr effect microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast “white light” supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains of two separate picosecond laser systems. The ability to independently tune the pump and probe wavelength enables themore » investigation of the influence of excitation energy on the optically induced electron spin dynamics in semiconductors. We demonstrate picosecond real-space imaging of the diffusive expansion of optically excited electron spin packets in a (110) GaAs quantum well sample to illustrate the capabilities of the instrument.« less

Observation of Ultrafast Magnon Dynamics in Antiferromagnetic Nickel Oxide by Optical Pump-Probe and Terahertz Time-Domain Spectroscopies

NASA Astrophysics Data System (ADS)

Kohmoto, T.; Moriyasu, T.; Wakabayashi, S.; Jinn, H.; Takahara, M.; Kakita, K.

2018-01-01

We have studied the ultrafast magnon dynamics in an antiferromagnetic 3d-transition-metal monoxide, nickel oxide (NiO), using optical pump-probe spectroscopy and terahertz time-domain spectroscopy (THz-TDS). THz damped magnon oscillations were observed in the Faraday rotation signal and in the transmitted THz electric field via optical pump-probe spectroscopy and THz-TDS, respectively. The magnon signals were observed in both the optical pump-probe spectroscopy and THz-TDS experiments, which shows that both Raman- and infrared-active modes are included in the NiO magnon modes. The magnon relaxation rate observed using THz-TDS was found to be almost constant up to the Néel temperature T N (= 523 K) and to increase abruptly near that temperature. This shows that temperature-independent spin-spin relaxation dominates up to T N . In our experiment, softening of the magnon frequency near T N was clearly observed. This result shows that the optical pump-probe spectroscopy and THz-TDS have high frequency resolution and a high signal to noise ratio in the THz region. We discuss the observed temperature dependence of the magnon frequencies using three different molecular field theories. The experimental results suggest that the biquadratic contribution of the exchange interaction plays an important role in the temperature dependence of the sublattice magnetization and the magnon frequency in cubic antiferromagnetic oxides.

Ultrafast magnetodynamics with free-electron lasers

NASA Astrophysics Data System (ADS)

Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

2018-02-01

The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

Relation between magnetization and Faraday angles produced by ultrafast spin-flip processes within the three-level Λ-type system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hinschberger, Y.; Lavoine, J. P.

2015-08-07

Ultrafast magneto-optical (MO) experiments constitute a powerful tool to explore the magnetization dynamics of diverse materials. Over the last decade, there have been many theoretical and experimental developments on this subject. However, the relation between the magnetization dynamics and the transient MO response still remains unclear. In this work, we calculate the magnetization of a material, as well as the magneto-optical rotation and ellipticity angles measured in a single-beam experiment. Then, we compare the magnetization to the MO response. The magnetic material is modeled by a three-level Λ-type system, which represents a simple model to describe MO effects induced bymore » an ultrafast laser pulse. Our calculations use the density matrix formalism, while the dynamics of the system is obtained by solving the Lindblad equation taking into account population relaxation and dephasing processes. Furthermore, we consider the Faraday rotation of the optical waves that simultaneously causes spin-flip. We show that the Faraday angles remain proportional to the magnetization only if the system has reached the equilibrium-state, and that this proportionality is directly related to the population and coherence decay rates. For the non-equilibrium situation, the previous proportionality relation is no longer valid. We show that our model is able to interpret some recent experimental results obtained in a single-pulse experiment. We further show that, after a critical pulse duration, the decrease of the ellipticity as a function of the absorbed energy is a characteristic of the system.« less

Role of the Heat Sink Layer Ta for Ultrafast Spin Dynamic Process in Amorphous TbFeCo Thin Films

NASA Astrophysics Data System (ADS)

Ren, Y.; Zhang, Z. Z.; Min, T.; Jin, Q. Y.

The ultrafast demagnetization processes (UDP) in Ta (t nm)/TbFeCo (20 nm) films have been studied using the time-resolved magneto-optical Kerr effect (TRMOKE). With a fixed pump fluence of 2 mJ/cm2, for the sample without a Ta underlayer (t=0nm), we observed the UDP showing a two-step decay behavior, with a relatively longer decay time (τ2) around 3.0 ps in the second step due to the equilibrium of spin-lattice relaxation following the 4f occupation. As a 10nm Ta layer is deposited, the two-step demagnetization still exists while τ2 decreases to ˜1.9ps. Nevertheless, the second-step decay (τ2=0ps) disappears as the Ta layer thickness is increased up to 20 nm, only the first-step UDP occurs within 500 fs, followed by a fast recovery process. The rapid magnetization recovery rate strongly depends on the pump fluence. We infer that the Ta layer provides conduction electrons involving the thermal equilibrium of spin-lattice interaction and serves as heat bath taking away energy from spins of TbFeCo alloy film in UDP.

High-frequency polarization dynamics in spin-lasers: pushing the limits

NASA Astrophysics Data System (ADS)

Gerhardt, Nils C.; Lindemann, Markus; Pusch, Tobias; Michalzik, Rainer; Hofmann, Martin R.

2017-09-01

While the high-frequency performance of conventional lasers is limited by the coupled carrier-photon dynamics, spin-polarized lasers have a high potential to overcome this limitation and to push the direct modulation bandwidth beyond 100 GHz. The key is to utilize the ultrafast polarization dynamics in spin-polarized vertical cavity surface-emitting lasers (spin-VCSELs) which is decoupled from the intensity dynamics and its fundamental limitations. The polarization dynamics in such devices, characterized by the polarization oscillation resonance frequency, is mainly determined by the amount of birefringence in the cavity. Using an approach for manipulating the birefringence via mechanical strain we were able to increase the polarization dynamics to resonance frequencies of more than 40 GHz. Up to now these values are only limited by the setup to induce birefringence and do not reflect any fundamental limitations. Taking our record results for the birefringence-induced mode splitting of more than 250 GHz into account, the concept has the potential to provide polarization modulation in spin-VCSELs with modulation frequencies far beyond 100 GHz. This makes them ideal devices for next-generation fast optical interconnects. In this paper we present experimental results for ultrafast polarization dynamics up to 50 GHz and compare them to numerical simulations.

Ultrafast optical control of individual quantum dot spin qubits.

PubMed

De Greve, Kristiaan; Press, David; McMahon, Peter L; Yamamoto, Yoshihisa

2013-09-01

Single spins in semiconductor quantum dots form a promising platform for solid-state quantum information processing. The spin-up and spin-down states of a single electron or hole, trapped inside a quantum dot, can represent a single qubit with a reasonably long decoherence time. The spin qubit can be optically coupled to excited (charged exciton) states that are also trapped in the quantum dot, which provides a mechanism to quickly initialize, manipulate and measure the spin state with optical pulses, and to interface between a stationary matter qubit and a 'flying' photonic qubit for quantum communication and distributed quantum information processing. The interaction of the spin qubit with light may be enhanced by placing the quantum dot inside a monolithic microcavity. An entire system, consisting of a two-dimensional array of quantum dots and a planar microcavity, may plausibly be constructed by modern semiconductor nano-fabrication technology and could offer a path toward chip-sized scalable quantum repeaters and quantum computers. This article reviews the recent experimental developments in optical control of single quantum dot spins for quantum information processing. We highlight demonstrations of a complete set of all-optical single-qubit operations on a single quantum dot spin: initialization, an arbitrary SU(2) gate, and measurement. We review the decoherence and dephasing mechanisms due to hyperfine interaction with the nuclear-spin bath, and show how the single-qubit operations can be combined to perform spin echo sequences that extend the qubit decoherence from a few nanoseconds to several microseconds, more than 5 orders of magnitude longer than the single-qubit gate time. Two-qubit coupling is discussed, both within a single chip by means of exchange coupling of nearby spins and optically induced geometric phases, as well as over longer-distances. Long-distance spin-spin entanglement can be generated if each spin can emit a photon that is entangled with the spin, and these photons are then interfered. We review recent work demonstrating entanglement between a stationary spin qubit and a flying photonic qubit. These experiments utilize the polarization- and frequency-dependent spontaneous emission from the lowest charged exciton state to single spin Zeeman sublevels.

Ultrafast giant magnetic cooling effect in ferromagnetic Co/Pt multilayers.

PubMed

Shim, Je-Ho; Ali Syed, Akbar; Kim, Chul-Hoon; Lee, Kyung Min; Park, Seung-Young; Jeong, Jong-Ryul; Kim, Dong-Hyun; Eon Kim, Dong

2017-10-06

The magnetic cooling effect originates from a large change in entropy by the forced magnetization alignment, which has long been considered to be utilized as an alternative environment-friendly cooling technology compared to conventional refrigeration. However, an ultimate timescale of the magnetic cooling effect has never been studied yet. Here, we report that a giant magnetic cooling (up to 200 K) phenomenon exists in the Co/Pt nano-multilayers on a femtosecond timescale during the photoinduced demagnetization and remagnetization, where the disordered spins are more rapidly aligned, and thus magnetically cooled, by the external magnetic field via the lattice-spin interaction in the multilayer system. These findings were obtained by the extensive analysis of time-resolved magneto-optical responses with systematic variation of laser fluence as well as external field strength and direction. Ultrafast giant magnetic cooling observed in the present study can enable a new avenue to the realization of ultrafast magnetic devices.The forced alignment of magnetic moments leads to a large change in entropy, which can be used to reduce the temperature of a material. Here, the authors show that this magnetic cooling effect occurs on a femtosecond time scale in cobalt-platinum nano-multilayers.

Ultrafast Time-Resolved Hard X-Ray Emission Spectroscopy on a Tabletop

NASA Astrophysics Data System (ADS)

Miaja-Avila, Luis; O'Neil, Galen C.; Joe, Young I.; Alpert, Bradley K.; Damrauer, Niels H.; Doriese, William B.; Fatur, Steven M.; Fowler, Joseph W.; Hilton, Gene C.; Jimenez, Ralph; Reintsema, Carl D.; Schmidt, Daniel R.; Silverman, Kevin L.; Swetz, Daniel S.; Tatsuno, Hideyuki; Ullom, Joel N.

2016-07-01

Experimental tools capable of monitoring both atomic and electronic structure on ultrafast (femtosecond to picosecond) time scales are needed for investigating photophysical processes fundamental to light harvesting, photocatalysis, energy and data storage, and optical display technologies. Time-resolved hard x-ray (>3 keV ) spectroscopies have proven valuable for these measurements due to their elemental specificity and sensitivity to geometric and electronic structures. Here, we present the first tabletop apparatus capable of performing time-resolved x-ray emission spectroscopy. The time resolution of the apparatus is better than 6 ps. By combining a compact laser-driven plasma source with a highly efficient array of microcalorimeter x-ray detectors, we are able to observe photoinduced spin changes in an archetypal polypyridyl iron complex [Fe (2 ,2'-bipyridine)3]2 + and accurately measure the lifetime of the quintet spin state. Our results demonstrate that ultrafast hard x-ray emission spectroscopy is no longer confined to large facilities and now can be performed in conventional laboratories with 10 times better time resolution than at synchrotrons. Our results are enabled, in part, by a 100- to 1000-fold increase in x-ray collection efficiency compared to current techniques.

Watching the dynamics of electrons and atoms at work in solar energy conversion.

PubMed

Canton, S E; Zhang, X; Liu, Y; Zhang, J; Pápai, M; Corani, A; Smeigh, A L; Smolentsev, G; Attenkofer, K; Jennings, G; Kurtz, C A; Li, F; Harlang, T; Vithanage, D; Chabera, P; Bordage, A; Sun, L; Ott, S; Wärnmark, K; Sundström, V

2015-01-01

The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium-cobalt dyads, which belong to the large family of donor-bridge-acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfer processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.

Control of Terahertz Emission by Ultrafast Spin-Charge Current Conversion at Rashba Interfaces

DOE PAGES

Jungfleisch, Matthias B.; Zhang, Qi; Zhang, Wei; ...

2018-05-18

Here, we show that a femtosecond spin-current pulse can generate terahertz (THz) transients at Rashba interfaces between two nonmagnetic materials. Our results unambiguously demonstrate the importance of the interface in this conversion process that we interpret in terms of the inverse Rashba Edelstein effect, in contrast to the THz emission in the bulk conversion process via the inverse spin-Hall effect. Furthermore, we show that at Rashba interfaces the THz-field amplitude can be controlled by the helicity of the light. The optical generation of electric photocurrents by these interfacial effects in the femtosecond regime will open up new opportunities in ultrafastmore » spintronics.« less

Control of Terahertz Emission by Ultrafast Spin-Charge Current Conversion at Rashba Interfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jungfleisch, Matthias B.; Zhang, Qi; Zhang, Wei

Here, we show that a femtosecond spin-current pulse can generate terahertz (THz) transients at Rashba interfaces between two nonmagnetic materials. Our results unambiguously demonstrate the importance of the interface in this conversion process that we interpret in terms of the inverse Rashba Edelstein effect, in contrast to the THz emission in the bulk conversion process via the inverse spin-Hall effect. Furthermore, we show that at Rashba interfaces the THz-field amplitude can be controlled by the helicity of the light. The optical generation of electric photocurrents by these interfacial effects in the femtosecond regime will open up new opportunities in ultrafastmore » spintronics.« less

Ultrafast generation of skyrmionic defects with vortex beams: Printing laser profiles on magnets

NASA Astrophysics Data System (ADS)

Fujita, Hiroyuki; Sato, Masahiro

2017-02-01

Controlling electric and magnetic properties of matter by laser beams is actively explored in the broad region of condensed matter physics, including spintronics and magneto-optics. Here we theoretically propose an application of optical and electron vortex beams carrying intrinsic orbital angular momentum to chiral ferro- and antiferromagnets. We analyze the time evolution of spins in chiral magnets under irradiation of vortex beams by using the stochastic Landau-Lifshitz-Gilbert equation. We show that beam-driven nonuniform temperature leads to a class of ring-shaped magnetic defects, what we call skyrmion multiplex, as well as conventional skyrmions. We discuss the proper beam parameters and the optimal way of applying the beams for the creation of these topological defects. Our findings provide an ultrafast scheme of generating topological magnetic defects in a way applicable to both metallic and insulating chiral (anti-) ferromagnets.

Terahertz emission from ultrafast spin and charge currents at a Rashba interface

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Qi; Jungfleisch, Matthias B.; Zhang, Wei

2017-01-01

Abstract: We demonstrate the efficient single-cycle THz emission from a Rashba interface, i.e., Ag/Bi, in a spintronic heterostructure. Different from the previously reported inversed spin Hall effect mechanism in bulk systems, the observed ultrafast spin-to-charge conversion in a 2D Rashba interface is due to the inversed Rashba-Edelstein effect.

Ultrafast universal quantum control of a quantum-dot charge qubit using Landau–Zener–Stückelberg interference

PubMed Central

Cao, Gang; Li, Hai-Ou; Tu, Tao; Wang, Li; Zhou, Cheng; Xiao, Ming; Guo, Guang-Can; Jiang, Hong-Wen; Guo, Guo-Ping

2013-01-01

A basic requirement for quantum information processing is the ability to universally control the state of a single qubit on timescales much shorter than the coherence time. Although ultrafast optical control of a single spin has been achieved in quantum dots, scaling up such methods remains a challenge. Here we demonstrate complete control of the quantum-dot charge qubit on the picosecond scale, orders of magnitude faster than the previously measured electrically controlled charge- or spin-based qubits. We observe tunable qubit dynamics in a charge-stability diagram, in a time domain, and in a pulse amplitude space of the driven pulse. The observations are well described by Landau–Zener–Stückelberg interference. These results establish the feasibility of a full set of all-electrical single-qubit operations. Although our experiment is carried out in a solid-state architecture, the technique is independent of the physical encoding of the quantum information and has the potential for wider applications. PMID:23360992

Ultrafast demagnetization at high temperatures

NASA Astrophysics Data System (ADS)

Hoveyda, F.; Hohenstein, E.; Judge, R.; Smadici, S.

2018-05-01

Time-resolved pump-probe measurements were made at variable heat accumulation in Co/Pd superlattices. Heat accumulation increases the baseline temperature and decreases the equilibrium magnetization. Transient ultrafast demagnetization first develops with higher fluence in parallel with strong equilibrium thermal spin fluctuations. The ultrafast demagnetization is then gradually removed as the equilibrium temperature approaches the Curie temperature. The transient magnetization time-dependence is well fit with the spin-flip scattering model.

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

PubMed

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-06-19

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification of transient, excited states, providing quantification of important parameters such as spin and orbital angular momenta as well as the energy gaps that separate electronic fine structure states. Ultrafast two-dimensional electronic spectroscopy (2DES) can be used to understand how these details influence state-to-state carrier dynamics. In combination, VTVH and 2DES methods can provide chemists with detailed information regarding the structure-dependent and state-specific flow of energy through metal nanoclusters. In this Account, we highlight recent advances toward understanding structure-dependent carrier dynamics for metals spanning the sub-nanometer to tens of nanometers length scale. We demonstrate the use of UCLEM methods for arresting interband scattering effects. For sub-nanometer thiol-protected nanoclusters, we discuss the effectiveness of VTVH for distinguishing state-specific radiative recombination originating from a gold core versus organometallic protecting layers. This state specificity is refined further using femtosecond 2DES and two-color methods to isolate so-called superatom state dynamics and vibrationally mediated spin-conversion and emission processes. Finally, we discuss prospects for merging VTVH and 2DES methods into a single platform.

Ultrafast Magnetism of Multi-component Ferromagnets and Ferrimagnets on the Time Scale of the Exchange Interaction

NASA Astrophysics Data System (ADS)

Radu, Ilie

2012-02-01

Revealing the ultimate speed limit at which magnetic order can be controlled, is a fundamental challenge of modern magnetism having far reaching implications for the magnetic recording industry [1]. Exchange interaction is the strongest force in magnetism, being ultimately responsible for ferromagnetic or antiferromagnetic spin order. How do spins react after being optically excited on a timescale of or even faster than the exchange interaction? Here, we demonstrate that femtosecond (fs) measurements of ferrimagnetic and ferromagnetic alloys using X-ray magnetic circular dichroism provide revolutionary new insights into the problem of ultrafast magnetism on timescales pertinent to the exchange interaction. In particular, we show that upon fs optical excitation the ultrafast spin reversal of GdFeCo - a material with antiferromagnetic coupling of spins - occurs via a transient ferromagnetic state [2]. The latter emerges due to different dynamics of the Gd and Fe magnetic moments: Gd switches within 1.5 ps while it takes only 300 fs for Fe. Thus, by using a single fs laser pulse one can force the spin system to evolve via an energetically unfavorable way and temporarily switch from an antiferromagnetic to a ferromagnetic type of ordering. In order to understand whether the observation of this temporarily decoupled and element-specific dynamics is a general phenomenon or just something strictly related to the case of ferrimagnetic GdFeCo, we have investigated the demagnetization of the archetypal ferromagnetic NiFe alloys. Essentially, we observe the same distinct magnetization dynamics of the constituent magnetic moments: Ni demagnetizes within ˜300 fs being much faster than the demagnetization of Fe of ˜800 fs. This distinct demagnetization behavior leads to an apparent decoupling of the Fe and Ni magnetic moments on a few hundreds of fs time scale, despite the strong exchange interaction of 260meV (˜16 fs) that couples them. These observations supported by atomistic simulations, present a novel concept of manipulating magnetic order on different classes of magnetic materials on timescales of the exchange interaction [3]. [4pt] [1] A. Kirilyuk, A.V. Kimel and Th. Rasing, Rev. Mod. Phys. 82, 2731 (2010). [0pt] [2] I. Radu et al., Nature 472, 205 (2011). [0pt] [3] I. Radu et al., submitted (2011).

Optical Manipulation and Detection of Emergent Phenomena in Topological Insulators

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gedik, Nuh

The three-dimensional topological insulator (TI) is a new quantum phase of matter that exhibits quantum-Hall-like properties, even in the absence of an external magnetic field. These materials are insulators in the bulk but have a topologically protected conducting state at the surface. Charge carriers on these surface states behave like a two-dimensional gas of massless helical Dirac fermions for which the spin is ideally locked perpendicular to the momentum. The purpose of this project is to probe the unique collective electronic behaviors of topological insulators by developing and using advanced time resolved spectroscopic techniques with state-of-the-art temporal and spatial resolutions.more » The nature of these materials requires development of specialized ultrafast techniques (such as time resolved ARPES that also has spin detection capability, ultrafast electron diffraction that has sub-100 fs time resolution and THz magneto-spectroscopy). The focus of this report is to detail our achievements in terms of establishing state of the art experimental facilities. Below, we will describe achievements under this award for the entire duration of five years. We will focus on detailing the development of ultrafast technqiues here. The details of the science that was done with these technqiues can be found in the publications referencing this grant.« less

Watching the dynamics of electrons and atoms at work in solar energy conversion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Canton, S. E.; Zhang, X.; Liu, Y.

2015-07-06

The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium–cobalt dyads, which belong to the large family of donor–bridge–acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfermore » processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.« less

Heat engine by exorcism of Maxwell Demon using spin angular momentum reservoir

NASA Astrophysics Data System (ADS)

Bedkihal, Salil; Wright, Jackson; Vaccaro, Joan; Gould, Tim

Landauer's erasure principle is a hallmark in thermodynamics and information theory. According to this principle, erasing one bit of information incurs a minimum energy cost. Recently, Vaccaro and Barnett (VB) have explored the role of multiple conserved quantities in memory erasure. They further illustrated that for the energy degenerate spin reservoirs, the cost of erasure can be solely in terms of spin angular momentum and no energy. Motivated by the VB erasure, in this work we propose a novel optical heat engine that operates under a single thermal reservoir and a spin angular momentum reservoir. The novel heat engine exploits ultrafast processes of phonon absorption to convert thermal phonon energy to coherent light. The entropy generated in this process then corresponds to a mixture of spin up and spin down populations of energy degenerate electronic ground states which acts as demon's memory. This information is then erased using a polarised spin reservoir that acts as an entropy sink. The proposed heat engines goes beyond the traditional Carnot engine.

Revealing giant internal magnetic fields due to spin fluctuations in magnetically doped colloidal nanocrystals

DOE PAGES

Rice, William D.; Liu, Wenyong; Baker, Thomas A.; ...

2015-11-23

Strong quantum confinement in semiconductors can compress the wavefunctions of band electrons and holes to nanometre-scale volumes, significantly enhancing interactions between themselves and individual dopants. In magnetically doped semiconductors, where paramagnetic dopants (such as Mn 2+, Co 2+ and so on) couple to band carriers via strong sp–d spin exchange, giant magneto-optical effects can therefore be realized in confined geometries using few or even single impurity spins. Importantly, however, thermodynamic spin fluctuations become increasingly relevant in this few-spin limit. In nanoscale volumes, the statistical √N fluctuations of N spins are expected to generate giant effective magnetic fields B eff, whichmore » should dramatically impact carrier spin dynamics, even in the absence of any applied field. In this paper, we directly and unambiguously reveal the large B eff that exist in Mn 2+-doped CdSe colloidal nanocrystals using ultrafast optical spectroscopy. At zero applied magnetic field, extremely rapid (300–600 GHz) spin precession of photoinjected electrons is observed, indicating B eff ~ 15-30 T for electrons. Precession frequencies exceed 2 THz in applied magnetic fields. Finally, these signals arise from electron precession about the random fields due to statistically incomplete cancellation of the embedded Mn 2+ moments, thereby revealing the initial coherent dynamics of magnetic polaron formation, and highlighting the importance of magnetization fluctuations on carrier spin dynamics in nanomaterials.« less

Effect of the spin-twist structure on the spin-wave dynamics in Fe{sub 55}Pt{sub 45}/Ni{sub 80}Fe{sub 20} exchange coupled bi-layers with varying Ni{sub 80}Fe{sub 20} thickness

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pal, Semanti; Barman, Saswati, E-mail: saswati@bose.res.in; Barman, Anjan, E-mail: abarman@bose.res.in

2014-05-07

We have investigated optically induced ultrafast magnetization dynamics of a series of Fe{sub 55}Pt{sub 45}/Ni{sub 80}Fe{sub 20} exchange spring bi-layers with varying Ni{sub 80}Fe{sub 20} thickness. Rich spin-wave spectra are observed; whose frequency shows a strong dependence on the Ni{sub 80}Fe{sub 20} layer thickness. Micromagnetic simulations based on a simplified magnetic microstructure were able to reproduce the experimental data qualitatively. The spin twist structure introduced in the Ni{sub 80}Fe{sub 20} layer gives rise to new modes in the composite system as opposed to the bare Ni{sub 80}Fe{sub 20} films.

Coherent Femtosecond Spectroscopy and Nonlinear Optical Imaging on the Nanoscale

NASA Astrophysics Data System (ADS)

Kravtsov, Vasily

Optical properties of many materials and macroscopic systems are defined by ultrafast dynamics of electronic, vibrational, and spin excitations localized on the nanoscale. Harnessing these excitations for material engineering, optical computing, and control of chemical reactions has been a long-standing goal in science and technology. However, it is challenging due to the lack of spectroscopic techniques that can resolve processes simultaneously on the nanometer spatial and femtosecond temporal scales. This thesis describes the fundamental principles, implementation, and experimental demonstration of a novel type of ultrafast microscopy based on the concept of adiabatic plasmonic nanofocusing. Simultaneous spatio-temporal resolution on a nanometer-femtosecond scale is achieved by using a near-field nonlinear optical response induced by ultrafast surface plasmon polaritons nanofocused on a metal tip. First, we study the surface plasmon response in metallic structures and evaluate its prospects and limitations for ultrafast near-field microscopy. Through plasmon emission-based spectroscopy, we investigate dephasing times and interplay between radiative and non-radiative decay rates of localized plasmons and their modification due to coupling. We identify a new regime of quantum plasmonic coupling, which limits the achievable spatial resolution to several angstroms but at the same time provides a potential channel for generating ultrafast electron currents at optical frequencies. Next, we study propagation of femtosecond wavepackets of surface plasmon polaritons on a metal tip. In time-domain interferometric measurements we detect group delays that correspond to slowing of the plasmon polaritons down to 20% of the speed of light at the tip apex. This provides direct experimental verification of the plasmonic nanofocusing mechanism and suggests enhanced nonlinear optical interactions at the tip apex. We then measure a plasmon-generated third-order nonlinear optical four-wave mixing response from the tip apex and investigate its microscopic mechanism. Our results reveal a significant contribution to the third order nonlinearity of plasmonic structures due to large near-field gradients associated with nanofocused plasmons. In combination with scanning probe imaging and femtosecond pulse shaping, the nanofocused four-wave mixing response provides a basis for a novel type of ultrafast optical microscopy on the nanoscale. We demonstrate its capabilities by nano-imaging the coherent dynamics of localized plasmonic modes in a rough gold film edge with simultaneous sub-50 nm spatial and sub-5 fs temporal resolution. We capture the coherent decay and extract the dephasing times of individual plasmonic modes. Lastly, we apply our technique to study nanoscale spatial heterogeneity of the nonlinear optical response in novel two-dimensional materials: monolayer and few-layer graphene. An enhanced four-wave mixing signal is revealed on the edges of graphene flakes. We investigate the mechanism of this enhancement by performing nano-imaging on a graphene field-effect transistor with the variable carrier density controlled by electrostatic gating.

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons.

PubMed

Bossini, D; Dal Conte, S; Hashimoto, Y; Secchi, A; Pisarev, R V; Rasing, Th; Cerullo, G; Kimel, A V

2016-02-05

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

Macrospin dynamics in antiferromagnets triggered by sub-20 femtosecond injection of nanomagnons

NASA Astrophysics Data System (ADS)

Bossini, D.; Dal Conte, S.; Hashimoto, Y.; Secchi, A.; Pisarev, R. V.; Rasing, Th.; Cerullo, G.; Kimel, A. V.

2016-02-01

The understanding of how the sub-nanoscale exchange interaction evolves in macroscale correlations and ordered phases of matter, such as magnetism and superconductivity, requires to bridging the quantum and classical worlds. This monumental challenge has so far only been achieved for systems close to their thermodynamical equilibrium. Here we follow in real time the ultrafast dynamics of the macroscale magnetic order parameter in the Heisenberg antiferromagnet KNiF3 triggered by the impulsive optical generation of spin excitations with the shortest possible nanometre wavelength and femtosecond period. Our magneto-optical pump-probe experiments also demonstrate the coherent manipulation of the phase and amplitude of these femtosecond nanomagnons, whose frequencies are defined by the exchange energy. These findings open up opportunities for fundamental research on the role of short-wavelength spin excitations in magnetism and strongly correlated materials; they also suggest that nanospintronics and nanomagnonics can employ coherently controllable spin waves with frequencies in the 20 THz domain.

Experimental demonstration of 55-fs spin canting in photoexcited iron nanoarrays

NASA Astrophysics Data System (ADS)

Ren, Yuhang; Lai, Wei; Cevher, Zehra; Gong, Yu; Zhang, G. P.

2017-02-01

As magnetic storage density approaches 1TB/in2, a grand challenge is looming as how to read/write such a huge amount of data within a reasonable time. The ultrafast optical manipulation of magnetization offers a solution, but little is known about the intrinsic speed limit of quantum spin switching. Here, we report that low-energy 50-fs laser pulses can induce spin canting in Fe nanoparticles within 55 fs, breaking the previous record by at least one order of magnitude. Both linearly and circularly polarized light can be used to tilt spins. In our model, the incident laser field first excites the orbital angular momentum, and through spin-orbit coupling, the spin cants out-of-plane and results in a distinctive diamond hysteresis loop. The spin canting time decreases with spin angular momentum. This spin canting is not limited to Fe nanoparticles and is also observed in Fe/Pt and Fe3O4 nanoparticles. Our results demonstrate the potential of magnetic nanostructures as a viable magnetic medium for high density and fast-switching magnetic storage devices.

Disparate ultrafast dynamics of itinerant and localized magnetic moments in gadolinium metal

PubMed Central

Frietsch, B.; Bowlan, J.; Carley, R.; Teichmann, M.; Wienholdt, S.; Hinzke, D.; Nowak, U.; Carva, K.; Oppeneer, P. M.; Weinelt, M.

2015-01-01

The Heisenberg–Dirac intra-atomic exchange coupling is responsible for the formation of the atomic spin moment and thus the strongest interaction in magnetism. Therefore, it is generally assumed that intra-atomic exchange leads to a quasi-instantaneous aligning process in the magnetic moment dynamics of spins in separate, on-site atomic orbitals. Following ultrashort optical excitation of gadolinium metal, we concurrently record in photoemission the 4f magnetic linear dichroism and 5d exchange splitting. Their dynamics differ by one order of magnitude, with decay constants of 14 versus 0.8 ps, respectively. Spin dynamics simulations based on an orbital-resolved Heisenberg Hamiltonian combined with first-principles calculations explain the particular dynamics of 5d and 4f spin moments well, and corroborate that the 5d exchange splitting traces closely the 5d spin-moment dynamics. Thus gadolinium shows disparate dynamics of the localized 4f and the itinerant 5d spin moments, demonstrating a breakdown of their intra-atomic exchange alignment on a picosecond timescale. PMID:26355196

Spin-vibronic quantum dynamics for ultrafast excited-state processes.

PubMed

Eng, Julien; Gourlaouen, Christophe; Gindensperger, Etienne; Daniel, Chantal

2015-03-17

Ultrafast intersystem crossing (ISC) processes coupled to nuclear relaxation and solvation dynamics play a central role in the photophysics and photochemistry of a wide range of transition metal complexes. These phenomena occurring within a few hundred femtoseconds are investigated experimentally by ultrafast picosecond and femtosecond transient absorption or luminescence spectroscopies, and optical laser pump-X-ray probe techniques using picosecond and femtosecond X-ray pulses. The interpretation of ultrafast structural changes, time-resolved spectra, quantum yields, and time scales of elementary processes or transient lifetimes needs robust theoretical tools combining state-of-the-art quantum chemistry and developments in quantum dynamics for solving the electronic and nuclear problems. Multimode molecular dynamics beyond the Born-Oppenheimer approximation has been successfully applied to many small polyatomic systems. Its application to large molecules containing a transition metal atom is still a challenge because of the nuclear dimensionality of the problem, the high density of electronic excited states, and the spin-orbit coupling effects. Rhenium(I) α-diimine carbonyl complexes, [Re(L)(CO)3(N,N)](n+) are thermally and photochemically robust and highly flexible synthetically. Structural variations of the N,N and L ligands affect the spectroscopy, the photophysics, and the photochemistry of these chromophores easily incorporated into a complex environment. Visible light absorption opens the route to a wide range of applications such as sensors, probes, or emissive labels for imaging biomolecules. Halide complexes [Re(X)(CO)3(bpy)] (X = Cl, Br, or I; bpy = 2,2'-bipyridine) exhibit complex electronic structure and large spin-orbit effects that do not correlate with the heavy atom effects. Indeed, the (1)MLCT → (3)MLCT intersystem crossing (ISC) kinetics is slower than in [Ru(bpy)3](2+) or [Fe(bpy)3](2+) despite the presence of a third-row transition metal. Counterintuitively, singlet excited-state lifetime increases on going from Cl (85 fs) to Br (128 fs) and to I (152 fs). Moreover, correlation between the Re-X stretching mode and the rate of ISC is observed. In this Account, we emphasize on the role of spin-vibronic coupling on the mechanism of ultrafast ISC put in evidence in [Re(Br)(CO)3(bpy)]. For this purpose, we have developed a model Hamiltonian for solving an 11 electronic excited states multimode problem including vibronic and SO coupling within the linear vibronic coupling (LVC) approximation and the assumption of harmonic potentials. The presence of a central metal atom coupled to rigid ligands, such as α-diimine, ensures nuclear motion of small amplitudes and a priori justifies the use of the LVC model. The simulation of the ultrafast dynamics by wavepacket propagations using the multiconfiguration time-dependent Hartree (MCTDH) method is based on density functional theory (DFT), and its time-dependent extension to excited states (TD-DFT) electronic structure data. We believe that the interplay between time-resolved experiments and these pioneering simulations covering the first picoseconds and including spin-vibronic coupling will promote a number of quantum dynamical studies that will contribute to a better understanding of ultrafast processes in a wide range of organic and inorganic chromophores easily incorporated in biosystems or supramolecular devices for specific functions.

Development of extreme ultraviolet and soft x-ray multilayer optics for scientific studies with femtosecond/attosecond sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aquila, Andrew Lee

The development of multilayer optics for extreme ultraviolet (EUV) radiation has led to advancements in many areas of science and technology, including materials studies, EUV lithography, water window microscopy, plasma imaging, and orbiting solar physics imaging. Recent developments in femtosecond and attosecond EUV pulse generation from sources such as high harmonic generation lasers, combined with the elemental and chemical specificity provided by EUV radiation, are opening new opportunities to study fundamental dynamic processes in materials. Critical to these efforts is the design and fabrication of multilayer optics to transport, focus, shape and image these ultra-fast pulses This thesis describes themore » design, fabrication, characterization, and application of multilayer optics for EUV femtosecond and attosecond scientific studies. Multilayer mirrors for bandwidth control, pulse shaping and compression, tri-material multilayers, and multilayers for polarization control are described. Characterization of multilayer optics, including measurement of material optical constants, reflectivity of multilayer mirrors, and metrology of reflected phases of the multilayer, which is critical to maintaining pulse size and shape, were performed. Two applications of these multilayer mirrors are detailed in the thesis. In the first application, broad bandwidth multilayers were used to characterize and measure sub-100 attosecond pulses from a high harmonic generation source and was performed in collaboration with the Max-Planck institute for Quantum Optics and Ludwig- Maximilians University in Garching, Germany, with Professors Krausz and Kleineberg. In the second application, multilayer mirrors with polarization control are useful to study femtosecond spin dynamics in an ongoing collaboration with the T-REX group of Professor Parmigiani at Elettra in Trieste, Italy. As new ultrafast x-ray sources become available, for example free electron lasers, the multilayer designs described in this thesis can be extended to higher photon energies, and such designs can be used with those sources to enable new scientific studies, such as molecular bonding, phonon, and spin dynamics.« less

Direct characterization of photoinduced lattice dynamics in BaFe 2As 2

DOE PAGES

Gerber, S.; Kim, K. W.; Zhang, Y.; ...

2015-06-08

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe 2As 2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent latticemore » dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.« less

Direct characterization of photoinduced lattice dynamics in BaFe2As2

PubMed Central

Gerber, S.; Kim, K. W.; Zhang, Y.; Zhu, D.; Plonka, N.; Yi, M.; Dakovski, G. L.; Leuenberger, D.; Kirchmann, P.S.; Moore, R. G.; Chollet, M.; Glownia, J. M.; Feng, Y.; Lee, J.-S.; Mehta, A.; Kemper, A. F.; Wolf, T.; Chuang, Y.-D.; Hussain, Z.; Kao, C.-C.; Moritz, B.; Shen, Z.-X.; Devereaux, T. P.; Lee, W.-S.

2015-01-01

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands. PMID:26051704

THz-driven demagnetization with perpendicular magnetic anisotropy: towards ultrafast ballistic switching

NASA Astrophysics Data System (ADS)

Polley, Debanjan; Pancaldi, Matteo; Hudl, Matthias; Vavassori, Paolo; Urazhdin, Sergei; Bonetti, Stefano

2018-02-01

We study THz-driven spin dynamics in thin CoPt films with perpendicular magnetic anisotropy. Femtosecond magneto-optical Kerr effect measurements show that demagnetization amplitude of about 1% can be achieved with a peak THz electric field of 300 kV cm-1, and a corresponding peak magnetic field of 0.1 T. The effect is more than an order of magnitude larger than observed in samples with easy-plane anisotropy irradiated with the same field strength. We also utilize finite-element simulations to design a meta-material structure that can enhance the THz magnetic field by more than an order of magnitude, over an area of several tens of square micrometers. Magnetic fields exceeding 1 Tesla, generated in such meta-materials with the available laser-based THz sources, are expected to produce full magnetization reversal via ultrafast ballistic precession driven by the THz radiation. Our results demonstrate the possibility of table-top ultrafast magnetization reversal induced by THz radiation.

Vibronically coherent ultrafast triplet-pair formation and subsequent thermally activated dissociation control efficient endothermic singlet fission

NASA Astrophysics Data System (ADS)

Stern, Hannah L.; Cheminal, Alexandre; Yost, Shane R.; Broch, Katharina; Bayliss, Sam L.; Chen, Kai; Tabachnyk, Maxim; Thorley, Karl; Greenham, Neil; Hodgkiss, Justin M.; Anthony, John; Head-Gordon, Martin; Musser, Andrew J.; Rao, Akshay; Friend, Richard H.

2017-12-01

Singlet exciton fission (SF), the conversion of one spin-singlet exciton (S1) into two spin-triplet excitons (T1), could provide a means to overcome the Shockley-Queisser limit in photovoltaics. SF as measured by the decay of S1 has been shown to occur efficiently and independently of temperature, even when the energy of S1 is as much as 200 meV less than that of 2T1. Here we study films of triisopropylsilyltetracene using transient optical spectroscopy and show that the triplet pair state (TT), which has been proposed to mediate singlet fission, forms on ultrafast timescales (in 300 fs) and that its formation is mediated by the strong coupling of electronic and vibrational degrees of freedom. This is followed by a slower loss of singlet character as the excitation evolves to become only TT. We observe the TT to be thermally dissociated on 10-100 ns timescales to form free triplets. This provides a model for 'temperature-independent' efficient TT formation and thermally activated TT separation.

Coherent energy scale revealed by ultrafast dynamics of UX3 (X = Al, Sn, Ga) single crystals

NASA Astrophysics Data System (ADS)

Nair, Saritha K.; Zhu, J.-X.; Sarrao, J. L.; Taylor, A. J.; Chia, Elbert E. M.

2012-09-01

The temperature dependence of relaxation dynamics of UX3 (X = Al, Ga, Sn) compounds is studied using the time-resolved pump-probe technique in reflectance geometry. For UGa3, our data are consistent with the formation of a spin density wave gap as evidenced from the quasidivergence of the relaxation time τ near the Néel temperature TN. For UAl3 and USn3, the relaxation dynamics shows a change from single-exponential to two-exponential behavior below a particular temperature, suggestive of coherence formation of the 5f electrons with the conduction band electrons. This particular temperature can be attributed to the spin fluctuation temperature Tsf, a measure of the strength of Kondo coherence. Our Tsf is consistent with other data such as resistivity and susceptibility measurements. The temperature dependence of the relaxation amplitude and time of UAl3 and USn3 were also fitted by the Rothwarf-Taylor model. Our results show that ultrafast optical spectroscopy is sensitive to c-f Kondo hybridization in the f-electron systems.

Demonstrating ultrafast polarization dynamics in spin-VCSELs

NASA Astrophysics Data System (ADS)

Lindemann, Markus; Pusch, Tobias; Michalzik, Rainer; Gerhardt, Nils C.; Hofmann, Martin R.

2018-02-01

Vertical-cavity surface-emitting lasers (VCSELs) are used for short-haul optical data transmission with increasing bit rates. The optimization involves both enhanced device designs and the use of higher-order modulation formats. In order to improve the modulation bandwidth substantially, the presented work employs spin-pumped VCSELs (spin-VCSELs) and their polarization dynamics instead of relying on intensity-modulated devices. In spin-VCSELs, the polarization state of the emitted light is controllable via spin injection. By optical spin pumping a single-mode VCSEL is forced to emit light composed of both orthogonal linearly polarized fundamental modes. The frequencies of these two modes differ slightly by a value determined by the cavity birefringence. As a result, the circular polarization degree oscillates with their beat frequency, i.e., with the birefringence-induced mode splitting. We used this phenomenon to show so-called polarization oscillations, which are generated by pulsed spin injection. Their frequency represents the polarization dynamics resonance frequency and can be tuned over a wide range via the birefringence, nearly independent from any other laser parameter. In previous work we demonstrated a maximum birefringence-induced mode splitting of more than 250 GHz. In this work, compared to previous publications, we show an almost doubled polarization oscillation frequency of more than 80 GHz. Furthermore, we discuss concepts to achieve even higher values far above 100 GHz.

Femtosecond optical reflectivity measurements of lattice-mediated spin repulsions in photoexcited LaCoO3 thin films

NASA Astrophysics Data System (ADS)

Bielecki, J.; Rata, A. D.; Börjesson, L.

2014-01-01

We present results on the temperature dependence of ultrafast electron and lattice dynamics, measured with pump-probe transient reflectivity experiments, of an epitaxially grown LaCoO3 thin film under tensile strain. Probing spin-polarized transitions into the antibonding eg band provides a measure of the low-spin fraction, both as a function of temperature and time after photoexcitation. It is observed that femtosecond laser pulses destabilize the constant low-spin fraction (˜63%-64%) in equilibrium into a thermally activated state, driven by a subpicosecond change in spin gap Δ. From the time evolution of the low-spin fraction, it is possible to disentangle the thermal and lattice contributions to the spin state. A lattice mediated spin repulsion, identified as the governing factor determining the equilibrium spin state in thin-film LaCoO3, is observed. These results suggests that time-resolved spectroscopy is a sensitive probe of the spin state in LaCoO3 thin films, with the potential to bring forward quantitative insight into the complicated interplay between structure and spin state in LaCoO3.

A highly ordered mesostructured material containing regularly distributed phenols: preparation and characterization at a molecular level through ultra-fast magic angle spinning proton NMR spectroscopy.

PubMed

Roussey, Arthur; Gajan, David; Maishal, Tarun K; Mukerjee, Anhurada; Veyre, Laurent; Lesage, Anne; Emsley, Lyndon; Copéret, Christophe; Thieuleux, Chloé

2011-03-14

Highly ordered organic-inorganic mesostructured material containing regularly distributed phenols is synthesized by combining a direct synthesis of the functional material and a protection-deprotection strategy and characterized at a molecular level through ultra-fast magic angle spinning proton NMR spectroscopy.

Ultrafast Spin Crossover in [FeII (bpy)3 ]2+ : Revealing Two Competing Mechanisms by Extreme Ultraviolet Photoemission Spectroscopy.

PubMed

Moguilevski, Alexandre; Wilke, Martin; Grell, Gilbert; Bokarev, Sergey I; Aziz, Saadullah G; Engel, Nicholas; Raheem, Azhr A; Kühn, Oliver; Kiyan, Igor Yu; Aziz, Emad F

2017-03-03

Photoinduced spin-flip in Fe II complexes is an ultrafast phenomenon that has the potential to become an alternative to conventional processing and magnetic storage of information. Following the initial excitation by visible light into the singlet metal-to-ligand charge-transfer state, the electronic transition to the high-spin quintet state may undergo different pathways. Here we apply ultrafast XUV (extreme ultraviolet) photoemission spectroscopy to track the low-to-high spin dynamics in the aqueous iron tris-bipyridine complex, [Fe(bpy) 3 ] 2+ , by monitoring the transient electron density distribution among excited states with femtosecond time resolution. Aided by first-principles calculations, this approach enables us to reveal unambiguously both the sequential and direct de-excitation pathways from singlet to quintet state, with a branching ratio of 4.5:1. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Theory of spin and lattice wave dynamics excited by focused laser pulses

NASA Astrophysics Data System (ADS)

Shen, Ka; Bauer, Gerrit E. W.

2018-06-01

We develop a theory of spin wave dynamics excited by ultrafast focused laser pulses in a magnetic film. We take into account both the volume and surface spin wave modes in the presence of applied, dipolar and magnetic anisotropy fields and include the dependence on laser spot exposure size and magnetic damping. We show that the sound waves generated by local heating by an ultrafast focused laser pulse can excite a wide spectrum of spin waves (on top of a dominant magnon–phonon contribution). Good agreement with recent experiments supports the validity of the model.

Ultrafast superresolution fluorescence imaging with spinning disk confocal microscope optics.

PubMed

Hayashi, Shinichi; Okada, Yasushi

2015-05-01

Most current superresolution (SR) microscope techniques surpass the diffraction limit at the expense of temporal resolution, compromising their applications to live-cell imaging. Here we describe a new SR fluorescence microscope based on confocal microscope optics, which we name the spinning disk superresolution microscope (SDSRM). Theoretically, the SDSRM is equivalent to a structured illumination microscope (SIM) and achieves a spatial resolution of 120 nm, double that of the diffraction limit of wide-field fluorescence microscopy. However, the SDSRM is 10 times faster than a conventional SIM because SR signals are recovered by optical demodulation through the stripe pattern of the disk. Therefore a single SR image requires only a single averaged image through the rotating disk. On the basis of this theory, we modified a commercial spinning disk confocal microscope. The improved resolution around 120 nm was confirmed with biological samples. The rapid dynamics of micro-tubules, mitochondria, lysosomes, and endosomes were observed with temporal resolutions of 30-100 frames/s. Because our method requires only small optical modifications, it will enable an easy upgrade from an existing spinning disk confocal to a SR microscope for live-cell imaging. © 2015 Hayashi and Okada. This article is distributed by The American Society for Cell Biology under license from the author(s). Two months after publication it is available to the public under an Attribution–Noncommercial–Share Alike 3.0 Unported Creative Commons License (http://creativecommons.org/licenses/by-nc-sa/3.0).

Ultrafast magnetization reversal by picosecond electrical pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Yang; Wilson, Richard B.; Gorchon, Jon

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

Ultrafast magnetization reversal by picosecond electrical pulses

DOE PAGES

Yang, Yang; Wilson, Richard B.; Gorchon, Jon; ...

2017-11-03

The field of spintronics involves the study of both spin and charge transport in solid-state devices. Ultrafast magnetism involves the use of femtosecond laser pulses to manipulate magnetic order on subpicosecond time scales. Here, we unite these phenomena by using picosecond charge current pulses to rapidly excite conduction electrons in magnetic metals. We observe deterministic, repeatable ultrafast reversal of the magnetization of a GdFeCo thin film with a single sub–10-ps electrical pulse. The magnetization reverses in ~10 ps, which is more than one order of magnitude faster than any other electrically controlled magnetic switching, and demonstrates a fundamentally new electricalmore » switching mechanism that does not require spin-polarized currents or spin-transfer/orbit torques. The energy density required for switching is low, projecting to only 4 fJ needed to switch a (20 nm) 3 cell. This discovery introduces a new field of research into ultrafast charge current–driven spintronic phenomena and devices.« less

Ultrafast magneto-optical spectroscopy of GaMnAs (Invited Paper)

NASA Astrophysics Data System (ADS)

Heroux, Jean Benoit; Kojima, Eiji; Ino, Y.; Hashimoto, Y.; Katsumoto, Shingo; Iye, Yasushiro; Kuwata-Gonokami, Makoto

2005-04-01

Spin dynamics in the III-V dilute magnetic semiconductor GaMnAs is investigated by photo-induced demagnetization. Experimental results obtained from two different time-dependent characterization techniques - "two color-probe" magneto-optical Kerr effect (TR-MOKE) and mid-infrared differential transmittance -- are compared. Upon photo-excitation with a 100 fs, 3.1 eV light pulse, a long demagnetization time in the hundreds of picoseconds timescale is found by TR-MOKE, indicating a spin-dependent band structure in this material. In mid-infrared measurements, a positive increase of the differential transmittance is observed in the same time interval when the sample is cooled below its Currie temperature. It is shown that this mid-infrared absorption feature is directly related to ferromagnetism in this material. The magnetism-related component of the broad DC mid-infrared absorption peak characteristic of this p-type material could be observed with this time-resolved measurement. Experimental results were simulated with a model describing the interaction between three thermal reservoirs (hole, spin and lattice) and taking thermal diffusion into account.

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel

PubMed Central

Tengdin, Phoebe; You, Wenjing; Chen, Cong; Shi, Xun; Zusin, Dmitriy; Zhang, Yingchao; Gentry, Christian; Blonsky, Adam; Keller, Mark; Oppeneer, Peter M.; Kapteyn, Henry C.; Tao, Zhensheng; Murnane, Margaret M.

2018-01-01

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization. PMID:29511738

Critical behavior within 20 fs drives the out-of-equilibrium laser-induced magnetic phase transition in nickel.

PubMed

Tengdin, Phoebe; You, Wenjing; Chen, Cong; Shi, Xun; Zusin, Dmitriy; Zhang, Yingchao; Gentry, Christian; Blonsky, Adam; Keller, Mark; Oppeneer, Peter M; Kapteyn, Henry C; Tao, Zhensheng; Murnane, Margaret M

2018-03-01

It has long been known that ferromagnets undergo a phase transition from ferromagnetic to paramagnetic at the Curie temperature, associated with critical phenomena such as a divergence in the heat capacity. A ferromagnet can also be transiently demagnetized by heating it with an ultrafast laser pulse. However, to date, the connection between out-of-equilibrium and equilibrium phase transitions, or how fast the out-of-equilibrium phase transitions can proceed, was not known. By combining time- and angle-resolved photoemission with time-resolved transverse magneto-optical Kerr spectroscopies, we show that the same critical behavior also governs the ultrafast magnetic phase transition in nickel. This is evidenced by several observations. First, we observe a divergence of the transient heat capacity of the electron spin system preceding material demagnetization. Second, when the electron temperature is transiently driven above the Curie temperature, we observe an extremely rapid change in the material response: The spin system absorbs sufficient energy within the first 20 fs to subsequently proceed through the phase transition, whereas demagnetization and the collapse of the exchange splitting occur on much longer, fluence-independent time scales of ~176 fs. Third, we find that the transient electron temperature alone dictates the magnetic response. Our results are important because they connect the out-of-equilibrium material behavior to the strongly coupled equilibrium behavior and uncover a new time scale in the process of ultrafast demagnetization.

Overview of selected seminal optical science and photonics processes in nature

NASA Astrophysics Data System (ADS)

Alfano, Robert R.

2016-03-01

This presentation gives an overview on some of seminal research in optical science, condensed matter physics, biophysics, biology, biomedical, nonlinear optics, and structure light propagation and interactions at CCNY and GTE Labs over past 46 years. The advent of ultrafast laser pulses with picosecond and femtosecond pulses and optical spectroscopy (label free native fluorescence and Raman) has led to unravel some of mysteries in the molecular world leading to breakthroughs in various areas of science and medicine. The following topics are discussed: white light continuum called now Supercontinuum (SC); first direct measurement of Optical Phonon's lifetimes; first observation of creation of daughter vibrations in time from excited mother vibration in liquids; first direct measurement of creation and decay of Spin Angular Momentum of electrons in GaAs where picosecond Circular Polarized Light carrying Optical Spin Angular Momentum is generated; Pulse break up into ballistic, snake and diffusive components in scattering media such as um beads and tissues; and use of optical spectroscopy for first cancer detection in label free tissues. Most recently, advances in Biomedical Optics showed that Tryptophan as a key biomarker for aggressive cancers; there are three new optical windows with the Golden window #3 the best for penetrating tissue from 1600 nm to 1800 nm; Complex light with OAM offers potential deeper tissue penetration and Resonance Raman excited using magic 532 nm wavelength in tissues.

Ultrafast Photo-Carrier Dynamics and Coherent Phonon Excitations in Topological Dirac Semimetal Cd3As2

NASA Astrophysics Data System (ADS)

Sun, Fei; Wu, Qiong; Wu, Yanling; Tian, Yichao; Shi, Youguo; Zhao, Jimin

Three dimensional (3D) topological Dirac semimetal has attracted growing research interest owing to its intriguing quantum properties such as high bulk carrier mobility and quantum spin Hall effects. However, so far, the ultrafast dynamics of a typical 3D topological Dirac semimetal, Cd3As2, as well as its coherent phonon has not been thoroughly investigated. Here we report the ultrafast dynamics of Cd3As2 by using femtosecond pump-probe spectroscopy. Two distinct relaxation processes was observed, with the lifetimes (at 5 K) of 2.4 ps and 18.6 ps, respectively. Variable temperature experiment from 5 K to 295 K also reveals signatures of phase transitions. Furthermore, coherent optical (8.1 meV) and acoustic (0.036 THz) phonon modes were generated and detected, respectively, with signatures of hybrid-excitation of the two modes. The National Basic Research Program of China (2012CB821402), the National Natural Science Foundation of China (11274372), and the External Cooperation Program of the Chinese Academy of Sciences (GJHZ1403).

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators.

PubMed

Battiato, Marco; Aguilera, Irene; Sánchez-Barriga, Jaime

2017-07-17

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin-orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized G W +Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron-electron and electron-phonon scatterings. Taking the prototypical insulator Bi 2 Te 3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron-electron and electron-phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials.

Ultrafast photophysics of transition metal complexes.

PubMed

Chergui, Majed

2015-03-17

The properties of transition metal complexes are interesting not only for their potential applications in solar energy conversion, OLEDs, molecular electronics, biology, photochemistry, etc. but also for their fascinating photophysical properties that call for a rethinking of fundamental concepts. With the advent of ultrafast spectroscopy over 25 years ago and, more particularly, with improvements in the past 10-15 years, a new area of study was opened that has led to insightful observations of the intramolecular relaxation processes such as internal conversion (IC), intersystem crossing (ISC), and intramolecular vibrational redistribution (IVR). Indeed, ultrafast optical spectroscopic tools, such as fluorescence up-conversion, show that in many cases, intramolecular relaxation processes can be extremely fast and even shorter than time scales of vibrations. In addition, more and more examples are appearing showing that ultrafast ISC rates do not scale with the magnitude of the metal spin-orbit coupling constant, that is, that there is no heavy-atom effect on ultrafast time scales. It appears that the structural dynamics of the system and the density of states play a crucial role therein. While optical spectroscopy delivers an insightful picture of electronic relaxation processes involving valence orbitals, the photophysics of metal complexes involves excitations that may be centered on the metal (called metal-centered or MC) or the ligand (called ligand-centered or LC) or involve a transition from one to the other or vice versa (called MLCT or LMCT). These excitations call for an element-specific probe of the photophysics, which is achieved by X-ray absorption spectroscopy. In this case, transitions from core orbitals to valence orbitals or higher allow probing the electronic structure changes induced by the optical excitation of the valence orbitals, while also delivering information about the geometrical rearrangement of the neighbor atoms around the atom of interest. With the emergence of new instruments such as X-ray free electron lasers (XFELs), it is now possible to perform ultrafast laser pump/X-ray emission probe experiments. In this case, one probes the density of occupied states. These core-level spectroscopies and other emerging ones, such as photoelectron spectroscopy of solutions, are delivering a hitherto unseen degree of detail into the photophysics of metal-based molecular complexes. In this Account, we will give examples of applications of the various methods listed above to address specific photophysical processes.

Laser-Induced Ultrafast Demagnetization: Femtomagnetism, a New Frontier?

NASA Astrophysics Data System (ADS)

Zhang, Guoping; Huebner, Wolfgang; Beaurepaire, Eric; Bigot, Jean-Yves

The conventional demagnetization process (spin precession, magnetic domain motion and rotation) is governed mainly by spin-lattice, magnetic dipole and Zeeman, and spin-spin interactions. It occurs on a timescale of nanoseconds. Technologically, much faster magnetization changes are always in great demand to improve data processing speed. Unfortunately, the present speed of magnetic devices is already at the limit of the conventional mechanism with little room left. Fortunately and unprecedentedly, recent experimental investigations have evidenced much faster magnetization dynamics which occurs on a femtosecond time scale: femtomagnetism. This novel spin dynamics has not been well-understood until now. This article reviews the current status of ultrafast spin dynamics and presents a perspective for future experimental and theoretical investigations.Present address: Department of Physics and Astronomy, The University of Tennessee at Knoxville, TN 37996-1200, USA; gpzhang@utk.edu

Gain-guided soliton fiber laser with high-quality rectangle spectrum for ultrafast time-stretch microscopy.

PubMed

Hu, Song; Yao, Jian; Liu, Meng; Luo, Ai-Ping; Luo, Zhi-Chao; Xu, Wen-Cheng

2016-05-16

The ultrafast time-stretch microscopy has been proposed to enhance the temporal resolution of a microscopy system. The optical source is a key component for ultrafast time-stretch microscopy system. Herein, we reported on the gain-guided soliton fiber laser with high-quality rectangle spectrum for ultrafast time-stretch microscopy. By virtue of the excellent characteristics of the gain-guided soliton, the output power and the 3-dB bandwidth of the stable mode-locked soliton could be up to 3 mW and 33.7 nm with a high-quality rectangle shape, respectively. With the proposed robust optical source, the ultrafast time-stretch microscopy with the 49.6 μm resolution and a scan rate of 11 MHz was achieved without the external optical amplification. The obtained results demonstrated that the gain-guided soliton fiber laser could be used as an alternative high-quality optical source for ultrafast time-stretch microscopy and will introduce some applications in fields such as biology, chemical, and optical sensing.

Ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials at optical communication range.

PubMed

Zhu, Yu; Hu, Xiaoyong; Fu, Yulan; Yang, Hong; Gong, Qihuang

2013-01-01

Actively all-optical tunable plasmon-induced transparency in metamaterials paves the way for achieving ultrahigh-speed quantum information processing chips. Unfortunately, up to now, very small experimental progress has been made for all-optical tunable plasmon-induced transparency in metamaterials in the visible and near-infrared range because of small third-order optical nonlinearity of conventional materials. The achieved operating pump intensity was as high as several GW/cm(2) order. Here, we report an ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials coated on polycrystalline indium-tin oxide layer at the optical communication range. Compared with previous reports, the threshold pump intensity is reduced by four orders of magnitude, while an ultrafast response time of picoseconds order is maintained. This work not only offers a way to constructing photonic materials with large nonlinearity and ultrafast response, but also opens up the possibility for realizing quantum solid chips and ultrafast integrated photonic devices based on metamaterials.

Ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials at optical communication range

PubMed Central

Zhu, Yu; Hu, Xiaoyong; Fu, Yulan; Yang, Hong; Gong, Qihuang

2013-01-01

Actively all-optical tunable plasmon-induced transparency in metamaterials paves the way for achieving ultrahigh-speed quantum information processing chips. Unfortunately, up to now, very small experimental progress has been made for all-optical tunable plasmon-induced transparency in metamaterials in the visible and near-infrared range because of small third-order optical nonlinearity of conventional materials. The achieved operating pump intensity was as high as several GW/cm2 order. Here, we report an ultralow-power and ultrafast all-optical tunable plasmon-induced transparency in metamaterials coated on polycrystalline indium-tin oxide layer at the optical communication range. Compared with previous reports, the threshold pump intensity is reduced by four orders of magnitude, while an ultrafast response time of picoseconds order is maintained. This work not only offers a way to constructing photonic materials with large nonlinearity and ultrafast response, but also opens up the possibility for realizing quantum solid chips and ultrafast integrated photonic devices based on metamaterials. PMID:23903825

Ultrafast magnon generation in an Fe film on Cu(100).

PubMed

Schmidt, A B; Pickel, M; Donath, M; Buczek, P; Ernst, A; Zhukov, V P; Echenique, P M; Sandratskii, L M; Chulkov, E V; Weinelt, M

2010-11-05

We report on a combined experimental and theoretical study of the spin-dependent relaxation processes in the electron system of an iron film on Cu(100). Spin-, time-, energy- and angle-resolved two-photon photoemission shows a strong characteristic dependence of the lifetime of photoexcited electrons on their spin and energy. Ab initio calculations as well as a many-body treatment corroborate that the observed properties are determined by relaxation processes involving magnon emission. Thereby we demonstrate that magnon emission by hot electrons occurs on the femtosecond time scale and thus provides a significant source of ultrafast spin-flip processes. Furthermore, engineering of the magnon spectrum paves the way for tuning the dynamic properties of magnetic materials.

Ultrafast probes of nonequilibrium hole spin relaxation in the ferromagnetic semiconductor GaMnAs

NASA Astrophysics Data System (ADS)

Patz, Aaron; Li, Tianqi; Liu, Xinyu; Furdyna, Jacek K.; Perakis, Ilias E.; Wang, Jigang

2015-04-01

We report direct measurements of hole spin lifetimes in ferromagnetic GaMnAs carried out by time- and polarization-resolved spectroscopy. Below the Curie temperature, ultrafast photoexcitation of GaMnAs with linearly polarized light is shown to create a nonequilibrium hole spin population via dynamical polarization of the holes through p -d exchange scattering with ferromagnetically ordered Mn spins. The system is then observed to relax in a distinct three-step recovery process: (i) a femtosecond hole spin relaxation, on the scale of 160-200 fs; (ii) a picosecond hole energy relaxation, on the scale of 1-2 ps; and (iii) a coherent, damped Mn spin precession with a period of 250 ps. The transient amplitude of the hole spin relaxation component diminishes with increasing temperature, directly following the ferromagnetic order of GaMnAs, while the hole energy amplitude shows negligible temperature change. Our results serve to establish the hole spin lifetimes in the ferromagnetic semiconductor GaMnAs, at the same time demonstrating a spectroscopic method for studying nonequilibrium hole spins in the presence of magnetic order and spin-exchange interaction.

Applications of ultrafast laser direct writing: from polarization control to data storage

NASA Astrophysics Data System (ADS)

Donko, A.; Gertus, T.; Brambilla, G.; Beresna, M.

2018-02-01

Ultrafast laser direct writing is a fascinating technology which emerged more than two decades from fundamental studies of material resistance to high-intensity optical fields. Its development saw the discovery of many puzzling phenomena and demonstration of useful applications. Today, ultrafast laser writing is seen as a technology with great potential and is rapidly entering the industrial environment. Whereas, less than 10 years ago, ultrafast lasers were still confined within the research labs. This talk will overview some of the unique features of ultrafast lasers and give examples of its applications in optical data storage, polarization control and optical fibers.

Ultrafast control and monitoring of material properties using terahertz pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bowlan, Pamela Renee

These are a set of slides on ultrafast control and monitoring of material properties using terahertz pulses. A few of the topics covered in these slides are: How fast is a femtosecond (fs), Different frequencies probe different properties of molecules or solids, What can a THz pulse do to a material, Ultrafast spectroscopy, Generating and measuring ultrashort THz pulses, Tracking ultrafast spin dynamics in antiferromagnets through spin wave resonances, Coherent two-dimensional THz spectroscopy, and Probing vibrational dynamics at a surface. Conclusions are: Coherent two-dimensional THz spectroscopy: a powerful approach for studying coherence and dynamics of low energy resonances. Applying thismore » to graphene we investigated the very strong THz light mater interaction which dominates over scattering. Useful for studying coupled excitations in multiferroics and monitoring chemical reactions. Also, THz-pump, SHG-probe spectoscopy: an ultrafast, surface sensitive probe of atomic-scale symmetry changes and nonlinear phonon dymanics. We are using this in Bi 2Se 3 to investigate the nonlinear surface phonon dynamics. This is potentially very useful for studying catalysis.« less

The complete optical oscilloscope

NASA Astrophysics Data System (ADS)

Lei, Cheng; Goda, Keisuke

2018-04-01

Observing ultrafast transient dynamics in optics is a challenging task. Two teams in Europe have now independently developed `optical oscilloscopes' that can capture both amplitude and phase information of ultrafast optical signals. Their schemes yield new insights into the nonlinear physics that takes place inside optical fibres.

Femtosecond optical characterization and applications in cadmium(manganese) telluride diluted magnetic semiconductors

NASA Astrophysics Data System (ADS)

Wang, Daozhi

This thesis is devoted to the optical characterization of Cd(Mn)Te single crystals. I present the studies of free-carrier dynamics and generation and detection of coherent acoustic phonons (CAPS) using time-resolved femtosecond pump-probe spectroscopy. The giant Faraday effect and ultrafast responsivity of Cd(Mn)Te to sub-picosecond electromagnetic transients are also demonstrated and discussed in detail. The first, few-picosecond-long electronic process after the initial optical excitation exhibits very distinct characteristic dependence on the excitation condition, and in case of Cd(Mn)Te, it has been attributed to the collective effects of band filling, band renormalization, and two-photon absorption. A closed-form, analytic expression for the differential reflectivity induced by the CAPs is derived based on the propagating-strain-pulse model and it accounts very well for our experimental observations. The accurate values of the Mn concentration and longitudinal sound velocity nu s in Cd(Mn)Te were obtained by fitting the data of the refractive index dependence on the probe wavelength to the Schubert model. In Cd 0.91Mn0.09Te, nus was found to be 3.6x103 m/s. Our comparison studies from the one-color and two-color experiments reveal that the intrinsic phonon lifetime in Cd(Mn)Te was at least on the order of nanoseconds, and the observed exponential damping of the CAP oscillations was due to the finite absorption depth of the probe light. Optically-induced electronic stress has been demonstrated to be the main generation mechanism of CAPs. We also present the giant Faraday effect in the Cd(Mn)Te and the spectra of the Verdet constant, which is mainly due to the exchange interaction between the Mn ions and band electrons. The spectral characteristics of the Verdet constant in Cd(Mn)Te exhibit very unique features compared to that in pure semiconductors. In our time-resolved sampling experiments at the room temperature, the response of the Cd(Mn)Te, particularly with low Mn concentrations, to the sub-picosecond electromagnetic pulses has been demonstrated for the first time and studied in detail. The physical origin of the ultrafast responsivity is shown to be the electro-optic (Pockels) effect, simultaneously excluding the magneto-optical (Faraday) effect due to the Mn-ion spin dynamics. The discrepancy between the absence of the low-frequency Pockels effect and the ultrafast sampling results, suggests that in Cd(Mn)Te crystals at low frequencies, the electric field component of the external electromagnetic transients is screened by the free carriers (holes). At very high (THz) frequencies, tested by our sampling experiment, Mn spins are too slow to respond and we observe the very large Pockels effect in Cd(Mn)Te crystals.

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI.

PubMed

Gutt, C; Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Raimondi, L; Nikolov, I P; Kiskinova, M; Jaiswal, S; Jakob, G; Kläui, M; Zabel, H; Pietsch, U

2017-09-01

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M 2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q -resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Q z , we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Effect of additional optical pumping injection into the ground-state ensemble on the gain and the phase recovery acceleration of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho

2014-02-01

The effect of additional optical pumping injection into the ground-state ensemble on the ultrafast gain and the phase recovery dynamics of electrically-driven quantum-dot semiconductor optical amplifiers is numerically investigated by solving 1088 coupled rate equations. The ultrafast gain and the phase recovery responses are calculated with respect to the additional optical pumping power. Increasing the additional optical pumping power can significantly accelerate the ultrafast phase recovery, which cannot be done by increasing the injection current density.

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

DOE PAGES

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; ...

2017-05-24

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born–Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersionmore » of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.« less

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching

NASA Astrophysics Data System (ADS)

Lemke, Henrik T.; Kjær, Kasper S.; Hartsock, Robert; van Driel, Tim B.; Chollet, Matthieu; Glownia, James M.; Song, Sanghoon; Zhu, Diling; Pace, Elisabetta; Matar, Samir F.; Nielsen, Martin M.; Benfatto, Maurizio; Gaffney, Kelly J.; Collet, Eric; Cammarata, Marco

2017-05-01

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.

Chirped pulse digital holography for measuring the sequence of ultrafast optical wavefronts

NASA Astrophysics Data System (ADS)

Karasawa, Naoki

2018-04-01

Optical setups for measuring the sequence of ultrafast optical wavefronts using a chirped pulse as a reference wave in digital holography are proposed and analyzed. In this method, multiple ultrafast object pulses are used to probe the temporal evolution of ultrafast phenomena and they are interfered with a chirped reference wave to record a digital hologram. Wavefronts at different times can be reconstructed separately from the recorded hologram when the reference pulse can be treated as a quasi-monochromatic wave during the pulse width of each object pulse. The feasibility of this method is demonstrated by numerical simulation.

Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators

PubMed Central

Battiato, Marco; Sánchez-Barriga, Jaime

2017-01-01

Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin–orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized GW+Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron–electron and electron–phonon scatterings. Taking the prototypical insulator Bi2Te3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron–electron and electron–phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials. PMID:28773171

Ultrafast magnetic vortex core switching driven by the topological inverse Faraday effect.

PubMed

Taguchi, Katsuhisa; Ohe, Jun-ichiro; Tatara, Gen

2012-09-21

We present a theoretical discovery of an unconventional mechanism of inverse Faraday effect which acts selectively on topological magnetic structures. The effect, topological inverse Faraday effect, is induced by the spin Berry's phase of the magnetic structure when a circularly polarized light is applied. Thus a spin-orbit interaction is not necessary unlike that in the conventional inverse Faraday effect. We demonstrate by numerical simulation that topological inverse Faraday effect realizes ultrafast switching of a magnetic vortex within a switching time of 150 ps without magnetic field.

Ultra-fast all-optical plasmon induced transparency in a metal–insulator–metal waveguide containing two Kerr nonlinear ring resonators

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-05-01

In this work, an ultra-fast all-optical plasmon induced transparency based on a metal–insulator–metal nanoplasmonic waveguide with two Kerr nonlinear ring resonators is studied. Two-dimensional simulations utilizing the finite-difference time-domain method are used to show an obvious optical bistability and significant switching mechanisms of the signal light by varying the pump-light intensity. The proposed all-optical switching based on plasmon induced transparency demonstrates femtosecond-scale feedback time (90 fs), meaning ultra-fast switching can be achieved. The presented all-optical switch may have potential significant applications in integrated optical circuits.

Quantum Dots

NASA Astrophysics Data System (ADS)

Tartakovskii, Alexander

2012-07-01

Part I. Nanostructure Design and Structural Properties of Epitaxially Grown Quantum Dots and Nanowires: 1. Growth of III/V semiconductor quantum dots C. Schneider, S. Hofling and A. Forchel; 2. Single semiconductor quantum dots in nanowires: growth, optics, and devices M. E. Reimer, N. Akopian, M. Barkelid, G. Bulgarini, R. Heeres, M. Hocevar, B. J. Witek, E. Bakkers and V. Zwiller; 3. Atomic scale analysis of self-assembled quantum dots by cross-sectional scanning tunneling microscopy and atom probe tomography J. G. Keizer and P. M. Koenraad; Part II. Manipulation of Individual Quantum States in Quantum Dots Using Optical Techniques: 4. Studies of the hole spin in self-assembled quantum dots using optical techniques B. D. Gerardot and R. J. Warburton; 5. Resonance fluorescence from a single quantum dot A. N. Vamivakas, C. Matthiesen, Y. Zhao, C.-Y. Lu and M. Atature; 6. Coherent control of quantum dot excitons using ultra-fast optical techniques A. J. Ramsay and A. M. Fox; 7. Optical probing of holes in quantum dot molecules: structure, symmetry, and spin M. F. Doty and J. I. Climente; Part III. Optical Properties of Quantum Dots in Photonic Cavities and Plasmon-Coupled Dots: 8. Deterministic light-matter coupling using single quantum dots P. Senellart; 9. Quantum dots in photonic crystal cavities A. Faraon, D. Englund, I. Fushman, A. Majumdar and J. Vukovic; 10. Photon statistics in quantum dot micropillar emission M. Asmann and M. Bayer; 11. Nanoplasmonics with colloidal quantum dots V. Temnov and U. Woggon; Part IV. Quantum Dot Nano-Laboratory: Magnetic Ions and Nuclear Spins in a Dot: 12. Dynamics and optical control of an individual Mn spin in a quantum dot L. Besombes, C. Le Gall, H. Boukari and H. Mariette; 13. Optical spectroscopy of InAs/GaAs quantum dots doped with a single Mn atom O. Krebs and A. Lemaitre; 14. Nuclear spin effects in quantum dot optics B. Urbaszek, B. Eble, T. Amand and X. Marie; Part V. Electron Transport in Quantum Dots Fabricated by Lithographic Techniques: III-V Semiconductors and Carbon: 15. Electrically controlling single spin coherence in semiconductor nanostructures Y. Dovzhenko, K. Wang, M. D. Schroer and J. R. Petta; 16. Theory of electron and nuclear spins in III-V semiconductor and carbon-based dots H. Ribeiro and G. Burkard; 17. Graphene quantum dots: transport experiments and local imaging S. Schnez, J. Guettinger, F. Molitor, C. Stampfer, M. Huefner, T. Ihn and K. Ensslin; Part VI. Single Dots for Future Telecommunications Applications: 18. Electrically operated entangled light sources based on quantum dots R. M. Stevenson, A. J. Bennett and A. J. Shields; 19. Deterministic single quantum dot cavities at telecommunication wavelengths D. Dalacu, K. Mnaymneh, J. Lapointe, G. C. Aers, P. J. Poole, R. L. Williams and S. Hughes; Index.

Ultrafast Microscopy of Spin-Momentum-Locked Surface Plasmon Polaritons.

PubMed

Dai, Yanan; Dąbrowski, Maciej; Apkarian, Vartkess A; Petek, Hrvoje

2018-06-26

Using two-photon photoemission electron microscopy (2P-PEEM) we image the polarization dependence of coupling and propagation of surface plasmon polaritons (SPPs) launched from edges of a triangular, micrometer size, single-crystalline Ag crystal by linearly or circularly polarized light. 2P-PEEM records interferences between the optical excitation field and SPPs it creates with nanofemto space-time resolution. Both the linearly and circularly polarized femtosecond light pulses excite spatially asymmetric 2PP yield distributions, which are imaged. We attribute the asymmetry for linearly polarized light to the relative alignments of the laser polarization and triangle edges, which affect the efficiency of excitation of the longitudinal component of the SPP field. For circular polarization, the asymmetry is caused by matching of the spin angular momenta (SAM) of light and the transverse SAM of SPPs. Moreover, we show that the interference patterns recorded in the 2P-PEEM images are cast by phase shifts and amplitudes for coupling of light into the longitudinal and transverse components of SPP fields. While the interference patterns depend on the excitation polarization, nanofemto movies show that the phase and group velocities of SPPs are independent of SAM of light in time-reversal invariant media. Simulations of the wave interference reproduce the polarization and spin-dependent coupling of optical pulses into SPPs.

Ultrafast Study of Dynamic Exchange Coupling in Ferromagnet/Oxide/Semiconductor Heterostructures

NASA Astrophysics Data System (ADS)

Ou, Yu-Sheng

Spintronics is the area of research that aims at utilizing the quantum mechanical spin degree of freedom of electrons in solid-state materials for information processing and data storage application. Since the discovery of the giant magnetoresistance, the field of spintronics has attracted lots of attention for its numerous potential advantages over contemporary electronics, such as less power consumption, high integration density and non-volatility. The realization of a spin battery, defined by the ability to create spin current without associated charge current, has been a long-standing goal in the field of spintronics. The demonstration of pure spin current in ferromagnet/nonmagnetic material hybrid structures by ferromagnetic resonance spin pumping has defined a thrilling direction for this field. As such, this dissertation targets at exploring the spin and magnetization dynamics in ferromagnet/oxide/semiconductor heterostructures (Fe/MgO/GaAs) using time-resolved optical pump-probe spectroscopy with the long-range goal of understanding the fundamentals of FMR-driven spin pumping. Fe/GaAs heterostructures are complex systems that contain multiple spin species, including paramagnetic spins (GaAs electrons), nuclear spins (Ga and As nuclei) and ferromagnetic spins (Fe). Optical pump-probe studies on their interplay have revealed a number of novel phenomena that has not been explored before. As such they will be the major focus of this dissertation. First, I will discuss the effect of interfacial exchange coupling on the GaAs free-carrier spin relaxation. Temperature- and field-dependent spin-resolved pump-probe studies reveal a strong correlation of the electron spin relaxation with carrier freeze-out, in quantitative agreement with a theoretical interpretation that at low temperatures the free-carrier spin lifetime is dominated by inhomogeneity in the local hyperfine field due to carrier localization. Second, we investigate the impact of tunnel barrier thickness on GaAs electron spin dynamics in Fe/MgO/GaAs heterostructures. Comparison of the Larmor frequency between samples with thick and thin MgO barriers reveals a four-fold variation in exchange coupling strength, and investigation of the spin lifetimes argues that inhomogeneity in the local hyperfine field dominates free-carrier spin relaxation across the entire range of barrier thickness. These results provide additional evidence to support the theory of hyperfine-dominated spin relaxation in GaAs. Third, we investigated the origin and dynamics of an emergent spin population by pump power and magnetic field dependent spin-resolved pump-probe studies. Power dependent study confirms its origin to be filling of electronic states in GaAs, and further field dependent studies reveal the impact of contact hyperfine coupling on the dynamics of electron spins occupying distinct electronic states. Beyond above works, we also pursue optical detection of dynamic spin pumping in Fe/MgO/GaAs heterostructures in parallel. I will discuss the development and progress that we have made toward this goal. This project can be simply divided into two phases. In the first phase, we focused on microwave excitation and optical detection of spin pumping. In the second phase, we focused on all-optical excitation and detection of spin pumping. A number of measurement strategies have been developed and executed in both stages to hunt for a spin pumping signal. I will discuss the preliminary data based upon them.

Controlled ultrafast transfer and stability degree of generalized coherent states of a kicked two-level ion

NASA Astrophysics Data System (ADS)

Chen, Hao; Kong, Chao; Hai, Wenhua

2018-06-01

We investigate quantum dynamics of a two-level ion trapped in the Lamb-Dicke regime of a δ -kicked optical lattice, based on the exact generalized coherent states rotated by a π / 2 pulse of Ramsey type experiment. The spatiotemporal evolutions of the spin-motion entangled states in different parameter regions are illustrated, and the parameter regions of different degrees of quantum stability described by the quantum fidelity are found. Time evolutions of the probability for the ion being in different pseudospin states reveal that the ultrafast entanglement generation and population transfers of the system can be analytically controlled by managing the laser pulses. The probability in an initially disentangled state shows periodic collapses (entanglement) and revivals (de-entanglement). Reduction of the stability degree results in enlarging the period of de-entanglement, while the instability and potential chaos will cause the sustained entanglement. The results could be justified experimentally in the existing setups and may be useful in engineering quantum dynamics for quantum information processing.

Ultrafast intersystem crossings in Fe-Co Prussian blue analogues

DOE Office of Scientific and Technical Information (OSTI.GOV)

van Veenendaal, Michel

Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co 3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt ( 4T 1) in 150-200 fs. In conclusion, strong oscillations inmore » spin-orbit coupling and the involvement of higher-lying quartets are found.« less

Ultrafast intersystem crossings in Fe-Co Prussian blue analogues

DOE PAGES

van Veenendaal, Michel

2017-07-27

Ultrafast spincrossover is studied in Fe-Co Prussian blue analogues using a dissipative quantum-mechanical model of a cobalt ion coupled to a breathing mode. All electronic interactions are treated on an equal footing. It is theoretically demonstrated that the divalent cobalt ion reaches 90% of the S = 3/2 value within 20 fs after photoexciting a low-spin Co 3+ ion by an iron-to-cobalt charge transfer. The doublet-to-quartet spin crossover is significantly faster than the oscillation period of the breathing mode. The system relaxes to the lowest manifold of divalent cobalt ( 4T 1) in 150-200 fs. In conclusion, strong oscillations inmore » spin-orbit coupling and the involvement of higher-lying quartets are found.« less

Broadband atomic-layer MoS₂ optical modulators for ultrafast pulse generations in the visible range.

PubMed

Zhang, Yuxia; Yu, Haohai; Zhang, Rui; Zhao, Gang; Zhang, Huaijin; Chen, Yanxue; Mei, Liangmo; Tonelli, Mauro; Wang, Jiyang

2017-02-01

Visible lasers are a fascinating regime, and their significance is illustrated by the 2014 Noble prizes in physics and chemistry. With the development of blue laser diodes (LDs), the LD-pumped solid-state visible lasers become a burgeoning direction today. Constrained by the scarce visible optical modulators, the solid-state ultrafast visible lasers are rarely realized. Based on the bandgap structure and optoelectronic properties of atomic-layer MoS₂, it can be proposed that MoS₂ has the potential as a visible optical modulator. Here, by originally revealing layer-dependent nonlinear absorption of the atomic-layer MoS₂ in the visible range, broadband atomic-layer MoS₂ optical modulators for the visible ultrafast pulse generation are developed and selected based on the proposed design criteria for novel two-dimensional (2D) optical modulators. By applying the selected MoS₂ optical modulators in the solid-state praseodymium lasers, broadband mode-locked ultrafast lasers from 522 to 639 nm are originally realized. We believe that this Letter should promote the development of visible ultrafast photonics and further applications of 2D optoelectronic materials.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, Arthur; Trebino, Rick P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques.

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

NASA Astrophysics Data System (ADS)

Gu, Mingqiang; Rondinelli, James M.

2016-04-01

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides.

PubMed

Gu, Mingqiang; Rondinelli, James M

2016-04-29

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.

Ultrafast band engineering and transient spin currents in antiferromagnetic oxides

DOE PAGES

Gu, Mingqiang; Rondinelli, James M.

2016-04-29

Here, we report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO 3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observedmore » in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO 3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices.« less

Ultrafast Band Engineering and Transient Spin Currents in Antiferromagnetic Oxides

PubMed Central

Gu, Mingqiang; Rondinelli, James M.

2016-01-01

We report a dynamic structure and band engineering strategy with experimental protocols to induce indirect-to-direct band gap transitions and coherently oscillating pure spin-currents in three-dimensional antiferromagnets (AFM) using selective phononic excitations. In the Mott insulator LaTiO3, we show that a photo-induced nonequilibrium phonon mode amplitude destroys the spin and orbitally degenerate ground state, reduces the band gap by 160 meV and renormalizes the carrier masses. The time scale of this process is a few hundreds of femtoseconds. Then in the hole-doped correlated metallic titanate, we show how pure spin-currents can be achieved to yield spin-polarizations exceeding those observed in classic semiconductors. Last, we demonstrate the generality of the approach by applying it to the non-orbitally degenerate AFM CaMnO3. These results advance our understanding of electron-lattice interactions in structures out-of-equilibrium and establish a rational framework for designing dynamic phases that may be exploited in ultrafast optoelectronic and optospintronic devices. PMID:27126354

Spin-orbit torque-driven skyrmion dynamics revealed by time-resolved X-ray microscopy

DOE PAGES

Woo, Seonghoon; Song, Kyung Mee; Han, Hee-Sung; ...

2017-05-24

Magnetic skyrmions are topologically protected spin textures with attractive properties suitable for high-density and low-power spintronic device applications. Much effort has been dedicated to understanding the dynamical behaviours of the magnetic skyrmions. However, experimental observation of the ultrafast dynamics of this chiral magnetic texture in real space, which is the hallmark of its quasiparticle nature, has so far remained elusive. Here, we report nanosecond-dynamics of a 100nm-diameter magnetic skyrmion during a current pulse application, using a time-resolved pump-probe soft X-ray imaging technique. We demonstrate that distinct dynamic excitation states of magnetic skyrmions, triggered by current-induced spin-orbit torques, can be reliablymore » tuned by changing the magnitude of spin-orbit torques. Our findings show that the dynamics of magnetic skyrmions can be controlled by the spin-orbit torque on the nanosecond time scale, which points to exciting opportunities for ultrafast and novel skyrmionic appl ications in the future.« less

Magnetic-field-induced crossover from the inverse Faraday effect to the optical orientation in EuTe

NASA Astrophysics Data System (ADS)

Pavlov, V. V.; Pisarev, R. V.; Nefedov, S. G.; Akimov, I. A.; Yakovlev, D. R.; Bayer, M.; Henriques, A. B.; Rappl, P. H. O.; Abramof, E.

2018-05-01

A time-resolved optical pump-probe technique has been applied for studying the ultrafast dynamics in the magnetic semiconductor EuTe near the absorption band gap. We show that application of external magnetic field up to 6 T results in crossover from the inverse Faraday effect taking place on the femtosecond time scale to the optical orientation phenomenon with an evolution in the picosecond time domain. We propose a model which includes both these processes, possessing different spectral and temporal properties. The circularly polarized optical pumping induces the electronic transition 4 f 7 5 d 0 → 4 f 6 5 d 1 forming the absorption band gap in EuTe. The observed crossover is related to a strong magnetic-field shift of the band gap in EuTe at low temperatures. It was found that manipulation of spin states on intrinsic defect levels takes place on a time scale of 19 ps in the applied magnetic field of 6 T.

The ``Music'' of Light: Optical Resonances for Fun and Profit

NASA Astrophysics Data System (ADS)

Beausoleil, Raymond

Moore's Law has set great expectations that the performance/price ratio of commercially available semiconductor devices will continue to improve exponentially at least until the end of this decade. But the physics of the metal wires that connect the transistors on a silicon chip already places stringent limits on the performance of integrated circuits, making their continued dramatic improvement highly unlikely. In this talk, I will introduce the basic concept of an optical resonance in a microscopic dielectric cavity in the context of the same type of spatial boundary conditions that give each musical instrument its unique sound. Then I will illustrate applications of these resonances to information technology in a variety of forms and functions using examples from my own laboratory at HP, such as chip-scale optical networks, quantum bits based on spins in diamond, and ultrafast optical switches that could become the foundation for a new generation of optical computers. Our goal is to conduct advanced research that could precipitate an ``optical Moore's Law'' and allow exponential performance gains to continue through the end of the next decade.

Apparatus and method for characterizing ultrafast polarization varying optical pulses

DOEpatents

Smirl, A.; Trebino, R.P.

1999-08-10

Practical techniques are described for characterizing ultrafast potentially ultraweak, ultrashort optical pulses. The techniques are particularly suited to the measurement of signals from nonlinear optical materials characterization experiments, whose signals are generally too weak for full characterization using conventional techniques. 2 figs.

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Beni, A.; Bogani, L.; Bussotti, L.; Dei, A.; Gentili, P. L.; Righini, R.

2005-01-01

The valence tautomerism of low-spin CoIII(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin CoII(Cat-N-BQ)2 that, secondly, reaches the chemical equilibrium with the reactant species.

Valley-selective photon-dressed states in transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

LaMountain, Trevor; Chen, Yen-Jung; Stanev, Teodor K.; Stern, Nathaniel P.

2018-02-01

When electronic excitations in a semiconductor interact with light, the relevant quasiparticles are hybrid lightmatter dressed states, or exciton-polaritons. In monolayer transition metal dichalcogenides, a class of 2D direct bandgap semiconductors, optical excitations selectively populate distinct momentum valleys with correlated spin projection. The combination of this spin-valley locking with photon dressed states can lead to new optical phenomena in these materials. We present spectroscopic measurements of valley-specific exciton-polaritons in monolayer 2D materials in distinct regimes. When a monolayer is embedded in a dielectric microcavity, strong coupling exciton-polaritons are achieved. Cavity-modified dynamics of the dressed states are inferred from emission. Polarization persists up to room temperature in monolayer MoS2, in contrast with bare material. We also show that distinct regimes of valley-polarized exciton-polaritons can be accessed with microcavity engineering by tuning system parameters such as cavity decay rate and exciton-photon coupling strength. Further, we report results showing that polarization-sensitive ultrafast spectroscopy can enable sensitive measurements of the valley optical Stark shift, a light-induced dressed state energy shift, in monolayer semiconductors such as WSe2 and MoS2. These findings demonstrate distinct approaches to manipulating the picosecond dynamics of valleysensitive dressed states in monolayer semiconductors.

Bosonic excitations and electron pairing in an electron-doped cuprate superconductor

NASA Astrophysics Data System (ADS)

Wang, M. C.; Yu, H. S.; Xiong, J.; Yang, Y.-F.; Luo, S. N.; Jin, K.; Qi, J.

2018-04-01

By applying ultrafast optical spectroscopy to electron-doped La1.9Ce0.1CuO4 ±δ , we discern a bosonic mode of electronic origin and provide the evolution of its coupling with the charge carriers as a function of temperature. Our results show that it has the strongest coupling strength near Tc and can fully account for the superconducting pairing. This mode can be associated with the two-dimensional antiferromagnetic spin correlations emerging below a critical temperature T† larger than Tc. Our work may help to establish a quantitative relation between bosonic excitations and superconducting pairing in electron-doped cuprates.

Roadmap on ultrafast optics

NASA Astrophysics Data System (ADS)

Reid, Derryck T.; Heyl, Christoph M.; Thomson, Robert R.; Trebino, Rick; Steinmeyer, Günter; Fielding, Helen H.; Holzwarth, Ronald; Zhang, Zhigang; Del'Haye, Pascal; Südmeyer, Thomas; Mourou, Gérard; Tajima, Toshiki; Faccio, Daniele; Harren, Frans J. M.; Cerullo, Giulio

2016-09-01

The year 2015 marked the 25th anniversary of modern ultrafast optics, since the demonstration of the first Kerr lens modelocked Ti:sapphire laser in 1990 (Spence et al 1990 Conf. on Lasers and Electro-Optics, CLEO, pp 619-20) heralded an explosion of scientific and engineering innovation. The impact of this disruptive technology extended well beyond the previous discipline boundaries of lasers, reaching into biology labs, manufacturing facilities, and even consumer healthcare and electronics. In recognition of such a milestone, this roadmap on Ultrafast Optics draws together articles from some of the key opinion leaders in the field to provide a freeze-frame of the state-of-the-art, while also attempting to forecast the technical and scientific paradigms which will define the field over the next 25 years. While no roadmap can be fully comprehensive, the thirteen articles here reflect the most exciting technical opportunities presented at the current time in Ultrafast Optics. Several articles examine the future landscape for ultrafast light sources, from practical solid-state/fiber lasers and Raman microresonators to exotic attosecond extreme ultraviolet and possibly even zeptosecond x-ray pulses. Others address the control and measurement challenges, requiring radical approaches to harness nonlinear effects such as filamentation and parametric generation, coupled with the question of how to most accurately characterise the field of ultrafast pulses simultaneously in space and time. Applications of ultrafast sources in materials processing, spectroscopy and time-resolved chemistry are also discussed, highlighting the improvements in performance possible by using lasers of higher peak power and repetition rate, or by exploiting the phase stability of emerging new frequency comb sources.

Polarization-dependent force driving the Eg mode in bismuth under optical excitation: comparison of first-principles theory with ultra-fast x-ray experiments

NASA Astrophysics Data System (ADS)

Fahy, Stephen; Murray, Eamonn

2015-03-01

Using first principles electronic structure methods, we calculate the induced force on the Eg (zone centre transverse optical) phonon mode in bismuth immediately after absorption of a ultrafast pulse of polarized light. To compare the results with recent ultra-fast, time-resolved x-ray diffraction experiments, we include the decay of the force due to carrier scattering, as measured in optical Raman scattering experiments, and simulate the optical absorption process, depth-dependent atomic driving forces, and x-ray diffraction in the experimental geometry. We find excellent agreement between the theoretical predictions and the observed oscillations of the x-ray diffraction signal, indicating that first-principles theory of optical absorption is well suited to the calculation of initial atomic driving forces in photo-excited materials following ultrafast excitation. This work is supported by Science Foundation Ireland (Grant No. 12/IA/1601) and EU Commission under the Marie Curie Incoming International Fellowships (Grant No. PIIF-GA-2012-329695).

Electron theory of fast and ultrafast dissipative magnetization dynamics.

PubMed

Fähnle, M; Illg, C

2011-12-14

For metallic magnets we review the experimental and electron-theoretical investigations of fast magnetization dynamics (on a timescale of ns to 100 ps) and of laser-pulse-induced ultrafast dynamics (few hundred fs). It is argued that for both situations the dominant contributions to the dissipative part of the dynamics arise from the excitation of electron-hole pairs and from the subsequent relaxation of these pairs by spin-dependent scattering processes, which transfer angular momentum to the lattice. By effective field theories (generalized breathing and bubbling Fermi-surface models) it is shown that the Gilbert equation of motion, which is often used to describe the fast dissipative magnetization dynamics, must be extended in several aspects. The basic assumptions of the Elliott-Yafet theory, which is often used to describe the ultrafast spin relaxation after laser-pulse irradiation, are discussed very critically. However, it is shown that for Ni this theory probably yields a value for the spin-relaxation time T(1) in good agreement with the experimental value. A relation between the quantity α characterizing the damping of the fast dynamics in simple situations and the time T(1) is derived. © 2011 IOP Publishing Ltd

Optimal control of laser-induced spin-orbit mediated ultrafast demagnetization

NASA Astrophysics Data System (ADS)

Elliott, P.; Krieger, K.; Dewhurst, J. K.; Sharma, S.; Gross, E. K. U.

2016-01-01

Laser induced ultrafast demagnetization is the process whereby the magnetic moment of a ferromagnetic material is seen to drop significantly on a timescale of 10-100 s of femtoseconds due to the application of a strong laser pulse. If this phenomenon can be harnessed for future technology, it offers the possibility for devices operating at speeds several orders of magnitude faster than at present. A key component to successful transfer of such a process to technology is the controllability of the process, i.e. that it can be tuned in order to overcome the practical and physical limitations imposed on the system. In this paper, we demonstrate that the spin-orbit mediated form of ultrafast demagnetization recently investigated (Krieger et al 2015 J. Chem. Theory Comput. 11 4870) by ab initio time-dependent density functional theory (TDDFT) can be controlled. To do so we use quantum optimal control theory (OCT) to couple our TDDFT simulations to the optimization machinery of OCT. We show that a laser pulse can be found which maximizes the loss of moment within a given time interval while subject to several practical and physical constraints. Furthermore we also include a constraint on the fluence of the laser pulses and find the optimal pulse that combines significant demagnetization with a desire for less powerful pulses. These calculations demonstrate optimal control is possible for spin-orbit mediated ultrafast demagnetization and lays the foundation for future optimizations/simulations which can incorporate even more constraints.

Complete Quantum Control of a Single Silicon-Vacancy Center in a Diamond Nanopillar

NASA Astrophysics Data System (ADS)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan-Kai; Dory, Constantin; Radulaski, Marina; Kelaita, Yousif; Shen, Zhi-Xun; Melosh, Nicholas A.; Chu, Steven; Vuckovic, Jelena

Coherent quantum control of a quantum bit (qubit) is an important step towards its use in a quantum network. SiV- center in diamond offers excellent physical qualities such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the fast spin manipulation and techniques to extend the spin coherence time are under active investigation. Here, we demonstrate full coherent control over the state of a single SiV- center in a diamond nanopillar using ultrafast optical pulses. The high quality of the chemical vapor deposition grown SiV- centers allows us to coherently manipulate and quasi-resonantly read out the state of the single SiV- center. Moreover, the SiV- centers being coherently controlled are integrated into diamond nanopillar arrays in a site-controlled, individually addressable manner with high yield, low strain, and high spectral stability, which paves the way for scalable on chip optically accessible quantum system in a quantum photonic network. Financial support is provided by the DOE Office of Basic Energy Sciences, Division of Materials Sciences through Stanford Institute for Materials and Energy Sciences (SIMES) under contract DE-AC02-76SF00515.

Resolving the role of femtosecond heated electrons in ultrafast spin dynamics.

PubMed

Mendil, J; Nieves, P; Chubykalo-Fesenko, O; Walowski, J; Santos, T; Pisana, S; Münzenberg, M

2014-02-05

Magnetization manipulation is essential for basic research and applications. A fundamental question is, how fast can the magnetization be reversed in nanoscale magnetic storage media. When subject to an ultrafast laser pulse, the speed of the magnetization dynamics depends on the nature of the energy transfer pathway. The order of the spin system can be effectively influenced through spin-flip processes mediated by hot electrons. It has been predicted that as electrons drive spins into the regime close to almost total demagnetization, characterized by a loss of ferromagnetic correlations near criticality, a second slower demagnetization process takes place after the initial fast drop of magnetization. By studying FePt, we unravel the fundamental role of the electronic structure. As the ferromagnet Fe becomes more noble in the FePt compound, the electronic structure is changed and the density of states around the Fermi level is reduced, thereby driving the spin correlations into the limit of critical fluctuations. We demonstrate the impact of the electrons and the ferromagnetic interactions, which allows a general insight into the mechanisms of spin dynamics when the ferromagnetic state is highly excited, and identifies possible recording speed limits in heat-assisted magnetization reversal.

Theoretical study on ultrafast intersystem crossing of chromium(III) acetylacetonate

NASA Astrophysics Data System (ADS)

Ando, Hideo; Iuchi, Satoru; Sato, Hirofumi

2012-05-01

In the relaxation process from the 4T2g state of chromium(III) acetylacetonate, CrIII(acac)3, ultrafast intersystem crossing (ISC) competes with vibrational relaxation (VR). This contradicts the conventional cascade model, where ISC rates are slower than VR ones. We hence investigate the relaxation process with quantum chemical calculations and excited-state wavepacket simulations to obtain clues about the origins of the ultrafast ISC. It is found that a potential energy curve of the 4T2g state crosses those of the 2T1g states near the Franck-Condon region and their spin-orbit couplings are strong. Consequently, ultrafast ISC between these states is observed in the wavepacket simulation.

Phase Recovery Acceleration of Quantum-Dot Semiconductor Optical Amplifiers by Optical Pumping to Quantum-Well Wetting Layer

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-11-01

We theoretically investigate the phase recovery acceleration of quantum-dot (QD) semiconductor optical amplifiers (SOAs) by means of the optical pump injection to the quantum-well (QW) wetting layer (WL). We compare the ultrafast gain and phase recovery responses of QD SOAs in either the electrical or the optical pumping scheme by numerically solving 1088 coupled rate equations. The ultrafast gain recovery responses on the order of sub-picosecond are nearly the same for the two pumping schemes. The ultrafast phase recovery is not significantly accelerated by increasing the electrical current density, but greatly improved by increasing the optical pumping power to the QW WL. Because the phase recovery time of QD SOAs with the optical pumping scheme can be reduced down to several picoseconds, the complete phase recovery can be achieved when consecutive pulse signals with a repetition rate of 100 GHz is injected.

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

NASA Astrophysics Data System (ADS)

Lejman, Mariusz; Vaudel, Gwenaelle; Infante, Ingrid C.; Chaban, Ievgeniia; Pezeril, Thomas; Edely, Mathieu; Nataf, Guillaume F.; Guennou, Mael; Kreisel, Jens; Gusev, Vitalyi E.; Dkhil, Brahim; Ruello, Pascal

2016-08-01

The ability to generate efficient giga-terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics.

Theoretical Investigation of Device Aspects of Semiconductor Superlattices.

DTIC Science & Technology

1983-09-01

n-i-p-i devices include bulk field effect transistors, ultrasensitive or ultrafast IR photodetectors , tunable light-emitting devices, and ultrafast...transistor4 ultrasensitive or ultrafast IR photodetectors , tunable light-emitt tg devices, and ultrafast optical modulators. Particularlylppealing...differential conductivity ( NDC ) ......................... 19 3.2.2. Spontaneous and stimulated FIR emission from interlayer transitions

Ultrafast spintronics roadmap: from femtosecond spin current pulses to terahertz non-uniform spin dynamics via nano-confined spin transfer torques (Conference Presentation)

NASA Astrophysics Data System (ADS)

Melnikov, Alexey; Razdolski, Ilya; Alekhin, Alexandr; Ilin, Nikita; Meyburg, Jan; Diesing, Detlef; Roddatis, Vladimir; Rungger, Ivan; Stamenova, Maria; Sanvito, Stefano; Bovensiepen, Uwe

2016-10-01

Further development of spintronics requires miniaturization and reduction of characteristic timescales of spin dynamics combining the nanometer spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the spin transfer torque (STT) exerted by ultrashort SC pulses on the FM open the time domain for studying STT fingerprint on spatially non-uniform magnetization dynamics. Using the sensitivity of magneto-induced second harmonic generation to SC, we develop technique for SC monitoring. With 20 fs resolution, we demonstrate the generation of 250 fs-long SC pulses in Fe/Au/Fe/MgO(001) structures. Their temporal profile indicates (i) nearly-ballistic hot electron transport in Au and (ii) that the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Together with strongly spin-dependent Fe/Au interface transmission calculated for these carriers, this suggests the non-thermal spin-dependent Seebeck effect dominating the generation of ultrashort SC pulses. The analysis of SC transmission/reflection at the Au/Fe interface shows that hot electron spins orthogonal to the Fe magnetization rotate gaining huge parallel (anti-parallel) projection in transmitted (reflected) SC. This is accompanied by a STT-induced perturbation of the magnetization localized at the interface, which excites the inhomogeneous high-frequency spin dynamics in the FM. Time-resolved magneto-optical studies reveal the excitation of several standing spin wave modes in the Fe film with their spectrum extending up to 0.6 THz and indicating the STT spatial confinement to 2 nm.

Polarization and dynamical properties of VCSELs-based photonic neuron subject to optical pulse injection

NASA Astrophysics Data System (ADS)

Xiang, Shuiying; Wen, Aijun; Zhang, Hao; Li, Jiafu; Guo, Xingxing; Shang, Lei; Lin, Lin

2016-11-01

The polarization-resolved nonlinear dynamics of vertical-cavity surface-emitting lasers (VCSELs) subject to orthogonally polarized optical pulse injection are investigated numerically based on the spin flip model. By extensive numerical bifurcation analysis, the responses dynamics of photonic neuron based on VCSELs under the arrival of external stimuli of orthogonally polarized optical pulse injection are mainly discussed. It is found that, several neuron-like dynamics, such as phasic spiking of a single abrupt large amplitude pulse followed with or without subthreshold oscillation, and tonic spiking with multiple periodic pulses, are successfully reproduced in the numerical model of VCSELs. Besides, the effects of stimuli strength, pump current, frequency detuning, as well as the linewidth enhancement factor on the neuron-like response dynamics are examined carefully. The operating parameters ranges corresponding to different neuron-like dynamics are further identified. Thus, the numerical model and simulation results are very useful and interesting for the ultrafast brain-inspired neuromorphic photonics systems based on VCSELs.

Polarization and Thickness Dependent Absorption Properties of Black Phosphorus: New Saturable Absorber for Ultrafast Pulse Generation

PubMed Central

Li, Diao; Jussila, Henri; Karvonen, Lasse; Ye, Guojun; Lipsanen, Harri; Chen, Xianhui; Sun, Zhipei

2015-01-01

Black phosphorus (BP) has recently been rediscovered as a new and interesting two-dimensional material due to its unique electronic and optical properties. Here, we study the linear and nonlinear optical properties of BP flakes. We observe that both the linear and nonlinear optical properties are anisotropic and can be tuned by the film thickness in BP, completely different from other typical two-dimensional layered materials (e.g., graphene and the most studied transition metal dichalcogenides). We then use the nonlinear optical properties of BP for ultrafast (pulse duration down to ~786 fs in mode-locking) and large-energy (pulse energy up to >18 nJ in Q-switching) pulse generation in fiber lasers at the near-infrared telecommunication band ~1.5 μm. We observe that the output of our BP based pulsed lasers is linearly polarized (with a degree-of-polarization ~98% in mode-locking, >99% in Q-switching, respectively) due to the anisotropic optical property of BP. Our results underscore the relatively large optical nonlinearity of BP with unique polarization and thickness dependence, and its potential for polarized optical pulse generation, paving the way to BP based nonlinear and ultrafast photonic applications (e.g., ultrafast all-optical polarization switches/modulators, frequency converters etc.). PMID:26514090

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

NASA Astrophysics Data System (ADS)

Gu, Min; Reid, Derryck; Ben-Yakar, Adela

2010-08-01

The use of light to explore biology can be traced to the first observations of tissue made with early microscopes in the mid-seventeenth century, and has today evolved into the discipline which we now know as biophotonics. This field encompasses a diverse range of activities, each of which shares the common theme of exploiting the interaction of light with biological material. With the rapid advancement of ultrafast optical technologies over the last few decades, ultrafast lasers have increasingly found applications in biophotonics, to the extent that the distinctive new field of ultrafast biophotonics has now emerged, where robust turnkey ultrafast laser systems are facilitating cutting-edge studies in the life sciences to take place in everyday laboratories. The broad spectral bandwidths, precision timing resolution, low coherence and high peak powers of ultrafast optical pulses provide unique opportunities for imaging and manipulating biological systems. Time-resolved studies of bio-molecular dynamics exploit the short pulse durations from such lasers, while other applications such as optical coherence tomography benefit from the broad optical bandwidths possible by using super-continuum generation and additionally allowing for high speed imaging with speeds as high as 47 000 scans per second. Continuing progress in laser-system technology is accelerating the adoption of ultrafast techniques across the life sciences, both in research laboratories and in clinical applications, such as laser-assisted in situ keratomileusis (LASIK) eye surgery. Revolutionizing the field of optical microscopy, two-photon excitation fluorescence (TPEF) microscopy has enabled higher spatial resolution with improved depth penetration into biological specimens. Advantages of this nonlinear optical process include: reduced photo-interactions, allowing for extensive imaging time periods; simultaneously exciting multiple fluorescent molecules with only one excitation wavelength; and reduced chromatic aberration effects. These extensive advantages have led to further exploration of nonlinear processes including second-harmonic generation (SHG) microscopy and third-harmonic generation (THG) microscopy. Second-harmonic generation has provided biologists with an extremely powerful tool for generating contrast in biological imaging, with the additional benefit of non-invasive three-dimensional imaging. The recent popularity of THG microscopy is largely due to the fact that three-dimensional imaging is achievable without the need for any labels, but rather relying on the intrinsic properties of the biological specimen itself. This optical nonlinear technique has attracted much attention recently from the biological community due to its non-invasive capabilities. Users of ultrafast lasers in the biological and medical fields are becoming a fast-growing community, employing pulse-shaping microscopy, resolution-enhancing microscopy techniques, linear and nonlinear micro-spectroscopy, functional deep-tissue imaging, optical coherence tomography, nonlinear fluorescence microscopy, molecular imaging and control, harmonic microscopy and femtosecond lifetime imaging, for cutting-edge research concerning the interaction of light with biological dynamics. The adaptability of ultrafast lasers to interact with a large array of materials through nonlinear excitation has enabled precise control of laser fluence allowing for highly localized material interactions, permitting micro-structured fabricated surfaces. The resultant multi-dimensional fabricated micro-structures are capable of replicating and/or manipulating microenvironments for controlled cell biology. In this special issue of Journal of Optics readers have a chance to view a collection of new contributions to the growing research field of ultrafast biophotonics. They are presented with recent advances in ultrafast technology applied to biological and medical investigations, where topics include advances in the visualization and identification of photo-reaction dynamics of biological functions under relevant physiological conditions, theoretically proposed imaging designs for obtaining super-resolved optical sectioned images in single exposures and fabricated micro-structured surfaces for biological micro-environments. We hope the collection will stimulate innovative new research in this growing field by showcasing new techniques for the visualization and manipulation of complex biological systems using linear and and nonlinear optical processes. Professor Min Gu would like to acknowledge Dr Betty Kouskousis for her contribution and support towards this editorial.

Quantum state-resolved probing of strong-field-ionized xenon atoms using femtosecond high-order harmonic transient absorption spectroscopy.

PubMed

Loh, Zhi-Heng; Khalil, Munira; Correa, Raoul E; Santra, Robin; Buth, Christian; Leone, Stephen R

2007-04-06

Femtosecond high-order harmonic transient absorption spectroscopy is used to resolve the complete |j,m quantum state distribution of Xe+ produced by optical strong-field ionization of Xe atoms at 800 nm. Probing at the Xe N4/5 edge yields a population distribution rhoj,|m| of rho3/2,1/2ratiorho1/2,1/2ratiorho3/2,3/2=75+/-6 :12+/-3 :13+/-6%. The result is compared to a tunnel ionization calculation with the inclusion of spin-orbit coupling, revealing nonadiabatic ionization behavior. The sub-50-fs time resolution paves the way for tabletop extreme ultraviolet absorption probing of ultrafast dynamics.

Optical properties of transiently-excited semiconductor hyperbolic metamaterials

DOE PAGES

Campione, Salvatore; Luk, Ting S.; Liu, Sheng; ...

2015-10-02

Ultrafast optical excitation of photocarriers has the potential to transform undoped semiconductor superlattices into semiconductor hyperbolic metamaterials (SHMs). In this paper, we investigate the optical properties associated with such ultrafast topological transitions. We first show reflectance, transmittance, and absorption under TE and TM plane wave incidence. In the unpumped state, the superlattice exhibits a frequency region with high reflectance (>80%) and a region with low reflectance (<1%) for both TE and TM polarizations over a wide range of incidence angles. In contrast, in the photopumped state, the reflectance for both frequencies and polarizations is very low (<1%) for a similarmore » range of angles. Interestingly, this system can function as an all-optical reflection switch on ultrafast timescales. Furthermore, for TM incidence and close to the epsilon-near-zero point of the longitudinal permittivity, directional perfect absorption on ultrafast timescales may also be achieved. Lastly, we discuss the onset of negative refraction in the photopumped state.« less

Model of ultrafast demagnetization driven by spin-orbit coupling in a photoexcited antiferromagnetic insulator Cr2O3

NASA Astrophysics Data System (ADS)

Guo, Feng; Zhang, Na; Jin, Wei; Chang, Jun

2017-06-01

We theoretically study the dynamic time evolution following laser pulse pumping in an antiferromagnetic insulator Cr2O3. From the photoexcited high-spin quartet states to the long-lived low-spin doublet states, the ultrafast demagnetization processes are investigated by solving the dissipative Schrödinger equation. We find that the demagnetization times are of the order of hundreds of femtoseconds, in good agreement with recent experiments. The switching times could be strongly reduced by properly tuning the energy gaps between the multiplet energy levels of Cr3+. Furthermore, the relaxation times also depend on the hybridization of atomic orbitals in the first photoexcited state. Our results suggest that the selective manipulation of the electronic structure by engineering stress-strain or chemical substitution allows effective control of the magnetic state switching in photoexcited insulating transition-metal oxides.

Time-dependent nonequilibrium soft x-ray response during a spin crossover

NASA Astrophysics Data System (ADS)

van Veenendaal, Michel

2018-03-01

A theoretical framework is developed for better understanding the time-dependent soft-x-ray response of dissipative quantum many-body systems. It is shown how x-ray absorption and resonant inelastic x-ray scattering (RIXS) at transition-metal L edges can provide insight into ultrafast intersystem crossings of importance for energy conversion, ultrafast magnetism, and catalysis. The photoinduced doublet-to-quartet spin crossover on cobalt in Fe-Co Prussian blue analogs is used as a model system to demonstrate how the x-ray response is affected by the nonequilibrium dynamics on a femtosecond time scale. Changes in local spin and symmetry and the underlying mechanism are reflected in strong broadenings, a collapse of clear selection rules during the intersystem crossing, fluctuations in the isotropic branching ratio in x-ray absorption, crystal-field collapse and/or oscillations, and time-dependent anti-Stokes processes in RIXS.

White light Z-scan measurements of ultrafast optical nonlinearity in reduced graphene oxide nanosheets in the 400–700 nm region

DOE Office of Scientific and Technical Information (OSTI.GOV)

Perumbilavil, Sreekanth; Sankar, Pranitha; Priya Rose, T.

Wavelength dispersion of optical power limiting is an important factor to be considered while designing potential optical limiters for laser safety applications. We report the observation of broadband, ultrafast optical limiting in reduced graphene oxide (rGO), measured by a single open aperture Z-scan using a white light continuum (WLC) source. WLC Z-scan is fast when the nonlinearity is to be measured over broad wavelength ranges, and it obviates the need for an ultrafast tunable laser making it cost-economic compared to conventional Z-scan. The nonlinearity arises from nondegenerate two-photon absorption, owing mostly to the crystallinity and extended π conjugation of rGO.

Ultrafast optical pulse convertor caused by oscillations of the energy level structure in the conjugated polymer poly(p-phenylenevinylene).

PubMed

Zhang, Yusong; Chen, Weikang; Lin, Zhe; Li, Sheng; George, Thomas F

2017-08-21

For a conjugated polymer irradiated by two optical pulses, the whole process of excitation, involving lattice oscillations, oscillations of the energy level structure, and evolution of the electron cloud, is investigated. Localization of the electron cloud appears in the first 100 fs of irradiation, which in turn induces vibrations of lattice of the polymer chain as well as oscillations of the band gap. These oscillations filter the absorption of the external optical field inversely and convert the original optical field to an ultrafast light field whose intensity varies with a certain period. Based on the mechanism, oscillations of the energy level structure, induced by the external excitation, can be designed as an ultrafast response optical convertor that is able to change the external optical pulse into a new effective light field with a certain oscillation period. This helps provide new insight into designing nanostructures for polymeric optoelectronics.

Ultrafast All-Optical Switching of Germanium-Based Flexible Metaphotonic Devices.

PubMed

Lim, Wen Xiang; Manjappa, Manukumara; Srivastava, Yogesh Kumar; Cong, Longqing; Kumar, Abhishek; MacDonald, Kevin F; Singh, Ranjan

2018-03-01

Incorporating semiconductors as active media into metamaterials offers opportunities for a wide range of dynamically switchable/tunable, technologically relevant optical functionalities enabled by strong, resonant light-matter interactions within the semiconductor. Here, a germanium-thin-film-based flexible metaphotonic device for ultrafast optical switching of terahertz radiation is experimentally demonstrated. A resonant transmission modulation depth of 90% is achieved, with an ultrafast full recovery time of 17 ps. An observed sub-picosecond decay constant of 670 fs is attributed to the presence of trap-assisted recombination sites in the thermally evaporated germanium film. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effect of wetting-layer density of states on the gain and phase recovery dynamics of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho; Yu, Bong-Ahn

2015-03-01

We numerically investigate the effect of the wetting-layer (WL) density of states on the gain and phase recovery dynamics of quantum-dot semiconductor optical amplifiers in both electrical and optical pumping schemes by solving 1088 coupled rate equations. The temporal variations of the ultrafast gain and phase recovery responses at the ground state (GS) are calculated as a function of the WL density of states. The ultrafast gain recovery responses do not significantly depend on the WL density of states in the electrical pumping scheme and the three optical pumping schemes such as the optical pumping to the WL, the optical pumping to the excited state ensemble, and the optical pumping to the GS ensemble. The ultrafast phase recovery responses are also not significantly affected by the WL density of states except the optical pumping to the WL, where the phase recovery component caused by the WL becomes slowed down as the WL density of states increases.

Femtosecond timing measurement and control using ultrafast organic thin films

NASA Astrophysics Data System (ADS)

Naruse, Makoto; Mitsu, Hiroyuki; Furuki, Makoto; Iwasa, Izumi; Sato, Yasuhiro; Tatsuura, Satoshi; Tian, Minquan

2003-12-01

We show a femtosecond timing measurement and control technique using a squarylium dye J-aggregate film, which is an organic thin film that acts as an ultrafast two-dimensional optical switch. Optical pulse timing is directly mapped to space-domain position on the film, and the large area and ultrafast response offer a femtosecond-resolved, large dynamic range, real-time, multichannel timing measurement capability. A timing fluctuation (jitter, wander, and skew) reduction architecture is presented and experimentally demonstrated.

Ultrafast NMR diffusion measurements exploiting chirp spin echoes.

PubMed

Ahola, Susanna; Mankinen, Otto; Telkki, Ville-Veikko

2017-04-01

Standard diffusion NMR measurements require the repetition of the experiment multiple times with varying gradient strength or diffusion delay. This makes the experiment time-consuming and restricts the use of hyperpolarized substances to boost sensitivity. We propose a novel single-scan diffusion experiment, which is based on spatial encoding of two-dimensional data, employing the spin-echoes created by two successive adiabatic frequency-swept chirp π pulses. The experiment is called ultrafast pulsed-field-gradient spin-echo (UF-PGSE). We present a rigorous derivation of the echo amplitude in the UF-PGSE experiment, justifying the theoretical basis of the method. The theory reveals also that the standard analysis of experimental data leads to a diffusion coefficient value overestimated by a few per cent. Although the overestimation is of the order of experimental error and thus insignificant in many practical applications, we propose that it can be compensated by a bipolar gradient version of the experiment, UF-BP-PGSE, or by corresponding stimulated-echo experiment, UF-BP-pulsed-field-gradient stimulated-echo. The latter also removes the effect of uniform background gradients. The experiments offer significant prospects for monitoring fast processes in real time as well as for increasing the sensitivity of experiments by several orders of magnitude by nuclear spin hyperpolarization. Furthermore, they can be applied as basic blocks in various ultrafast multidimensional Laplace NMR experiments. Copyright © 2016 John Wiley & Sons, Ltd. Copyright © 2016 John Wiley & Sons, Ltd.

Material processing with fiber based ultrafast pulse delivery

NASA Astrophysics Data System (ADS)

Baumbach, S.; Stockburger, R.; Führa, B.; Zoller, S.; Thum, S.; Moosmann, J.; Maier, D.; Kanal, F.; Russ, S.; Kaiser, E.; Budnicki, A.; Sutter, D. H.; Pricking, S.; Killi, A.

2018-02-01

We report on TRUMPF's ultrafast laser systems equipped with industrialized hollow core fiber laser light cables. Beam guidance in general by means of optical fibers, e.g. for multi kilowatt cw laser systems, has become an integral part of laser-based material processing. One advantage of fiber delivery, among others, is the mechanical separation between laser and processing head. An equally important benefit is given by the fact that the fiber end acts as an opto-mechanical fix-point close to successive optical elements in the processing head. Components like lenses, diffractive optical elements etc. can thus be designed towards higher efficiency which results in better material processing. These aspects gain increasing significance when the laser system operates in fundamental mode which is usually the case for ultrafast lasers. Through the last years beam guidance of ultrafast laser pulses by means of hollow core fiber technology established very rapidly. The combination of TRUMPF's long-term stable ultrafast laser sources, passive fiber coupling, connector and packaging forms a flexible and powerful system for laser based material processing well suited for an industrial environment. In this article we demonstrate common material processing applications with ultrafast lasers realized with TRUMPF's hollow core fiber delivery. The experimental results are contrasted and evaluated against conventional free space propagation in order to illustrate the performance of flexible ultrafast beam delivery.

Ultrafast electrical spectrum analyzer based on all-optical Fourier transform and temporal magnification.

PubMed

Duan, Yuhua; Chen, Liao; Zhou, Haidong; Zhou, Xi; Zhang, Chi; Zhang, Xinliang

2017-04-03

Real-time electrical spectrum analysis is of great significance for applications involving radio astronomy and electronic warfare, e.g. the dynamic spectrum monitoring of outer space signal, and the instantaneous capture of frequency from other electronic systems. However, conventional electrical spectrum analyzer (ESA) has limited operation speed and observation bandwidth due to the electronic bottleneck. Therefore, a variety of photonics-assisted methods have been extensively explored due to the bandwidth advantage of the optical domain. Alternatively, we proposed and experimentally demonstrated an ultrafast ESA based on all-optical Fourier transform and temporal magnification in this paper. The radio-frequency (RF) signal under test is temporally multiplexed to the spectrum of an ultrashort pulse, thus the frequency information is converted to the time axis. Moreover, since the bandwidth of this ultrashort pulse is far beyond that of the state-of-the-art photo-detector, a temporal magnification system is applied to stretch the time axis, and capture the RF spectrum with 1-GHz resolution. The observation bandwidth of this ultrafast ESA is over 20 GHz, limited by that of the electro-optic modulator. Since all the signal processing is in the optical domain, the acquisition frame rate can be as high as 50 MHz. This ultrafast ESA scheme can be further improved with better dispersive engineering, and is promising for some ultrafast spectral information acquisition applications.

Femtosecond Optical and X-Ray Measurement of the Semiconductor-to-Metal Transition in VO2

NASA Astrophysics Data System (ADS)

Cavalleri, Andrea; Toth, Csaba; Squier, Jeff; Siders, Craig; Raksi, Ferenc; Forget, Patrick; Kieffer, Jean-Claude

2001-03-01

While the use of ultrashort visible pulses allows access to ultrafast changes in the optical properties during phase transitions, measurement of the correlation between atomic movement and electronic rearrangement has proven more elusive. Here, we report on the conjunct measurement of ultrafast electronic and structural dynamics during a semiconductor-to-metal phase transition in VO2. Rearrangement of the unit cell from monoclinic to rutile (measured by ultrafast x-ray diffraction) is accompanied by a sharp increase in the electrical conductivity and perturbation of the optical properties (measured with ultrafast visible spectroscopy). Ultrafast x-ray diffraction experiments were performed using femtosecond bursts of Cu-Ka from a laser generated plasma source. A clear rise of the diffraction signal originating from the impulsively generated metallic phase was observable on the sub-picosecond timescale. Optical experiments were performed using time-resolved microscopy, providing temporally and spatially resolved measurements of the optical reflectivity at 800 nm. The data indicate that the reflectivity of the low-temperature semiconducting solid is driven to that of the equilibrium, high-temperature metallic phase within 400 fs after irradiation with a 50-fs laser pulse at fluences in excess of 10 mJ/cm2. In conclusion, the data presented in this contribution suggest that the semiconductor-to-metal transition in VO2 occurs within 500 fs after laser-irradiation. A nonthermal physical mechanism governs the re-arrangement.

Element-selective investigation of domain structure in CoPd and FePd alloys using small-angle soft X-ray scattering

NASA Astrophysics Data System (ADS)

Weier, C.; Adam, R.; Frömter, R.; Bach, J.; Winkler, G.; Kobs, A.; Oepen, H. P.; Grychtol, P.; Kapteyn, H. C.; Murnane, M. M.; Schneider, C. M.

2014-03-01

Recent optical pump-probe experiments on magnetic multilayers and alloys identified perpendicular spin superdiffusion as one of possible mechanisms responsible for femtosecond magnetization dynamics. On the other hand, no strong evidence for the ultrafast lateral spin transport has been reported, so far. To address this question, we studied magnetic domain structure of CoPd and FePd thin films using small-angle scattering of soft X-rays. By tuning the synchrotron-generated X-rays to the absorption edges of Fe or Co we recorded Fourier images of the magnetic domain structure corresponding to a chosen element. Applying in - situ magnetic fields resulted in pronounced rearrangement of domain structure that was clearly observed in scattering images. Our analysis of both the stand-alone, as well as magnetically coupled CoPd/FePd layers provides insight into the formation of domains under small magnetic field perturbations and pave the way to better understanding of transient changes expected in magneto-dynamic measurements.

Itinerant and localized magnetization dynamics in antiferromagnetic Ho

DOE PAGES

Rettig, L.; Dornes, C.; Thielemann-Kuhn, N.; ...

2016-06-21

Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L 3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Here, tuning the x-ray energy to the electric dipole (E1, 2p → 5d) or quadrupole (E2, 2p → 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3–τ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similarmore » spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f–5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magneto-striction leads to a transient shift of the magnetic satellite peak.« less

Microresonator-Based Optical Frequency Combs: A Time Domain Perspective

DTIC Science & Technology

2016-04-19

optics; ultrafast optics 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT 18. NUMBER OF PAGES 19a. NAME OF RESPONSIBLE PERSON a...generation at frequency spacings down to 25 GHz, in the range where convenient electronic detection is possible. (c) Our best Purdue microrings had...time domain measurements of the generated combs, leading to observation of novel, ultrafast dark pulse waveforms, have introduced new structures such

40-Gbit/s all-optical circulating shift register with an inverter.

PubMed

Hall, K L; Donnelly, J P; Groves, S H; Fennelly, C I; Bailey, R J; Napoleone, A

1997-10-01

We report what is believed to be the first demonstration of an all-optical circulating shift register using an ultrafast nonlinear interferometer with a polarization-insensitive semiconductor optical amplifier as the nonlinear switching element. The device operates at 40 Gbits/s, to our knowledge the highest speed demonstrated to date. Also, the demonstration proves the cascadability of the ultrafast nonlinear interferometric switch.

Noncollinear generation of optical spatiotemporal solitons and application to ultrafast digital logic

NASA Astrophysics Data System (ADS)

Liu, Xiang; Beckwitt, Kale; Wise, Frank

2000-05-01

We demonstrate theoretically and experimentally that spatiotemporal solitons can be generated through noncollinear second-harmonic generation. The resulting Y geometry could be used to implement an optical AND gate with ultrafast, high-contrast operation but without sensitivity to the phases of the input pulses.

Electrically-driven GHz range ultrafast graphene light emitter (Conference Presentation)

NASA Astrophysics Data System (ADS)

Kim, Youngduck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Kim, Hyungsik; Nemilentsau, Andrei M.; Low, Tony; Taniguchi, Takashi; Watanabe, Kenji; Bae, Myung-Ho; Heinz, Tony F.; Englund, Dirk R.; Hone, James

2017-02-01

Ultrafast electrically driven light emitter is a critical component in the development of the high bandwidth free-space and on-chip optical communications. Traditional semiconductor based light sources for integration to photonic platform have therefore been heavily studied over the past decades. However, there are still challenges such as absence of monolithic on-chip light sources with high bandwidth density, large-scale integration, low-cost, small foot print, and complementary metal-oxide-semiconductor (CMOS) technology compatibility. Here, we demonstrate the first electrically driven ultrafast graphene light emitter that operate up to 10 GHz bandwidth and broadband range (400 1600 nm), which are possible due to the strong coupling of charge carriers in graphene and surface optical phonons in hBN allow the ultrafast energy and heat transfer. In addition, incorporation of atomically thin hexagonal boron nitride (hBN) encapsulation layers enable the stable and practical high performance even under the ambient condition. Therefore, electrically driven ultrafast graphene light emitters paves the way towards the realization of ultrahigh bandwidth density photonic integrated circuits and efficient optical communications networks.

Spin relaxation dynamics of holes in intrinsic GaAs quantum wells studied by transient circular dichromatic absorption spectroscopy at room temperature.

PubMed

Fang, Shaoyin; Zhu, Ruidan; Lai, Tianshu

2017-03-21

Spin relaxation dynamics of holes in intrinsic GaAs quantum wells is studied using time-resolved circular dichromatic absorption spectroscopy at room temperature. It is found that ultrafast dynamics is dominated by the cooperative contributions of band filling and many-body effects. The relative contribution of the two effects is opposite in strength for electrons and holes. As a result, transient circular dichromatic differential transmission (TCD-DT) with co- and cross-circularly polarized pump and probe presents different strength at several picosecond delay time. Ultrafast spin relaxation dynamics of excited holes is sensitively reflected in TCD-DT with cross-circularly polarized pump and probe. A model, including coherent artifact, thermalization of nonthermal carriers and the cooperative contribution of band filling and many-body effects, is developed, and used to fit TCD-DT with cross-circularly polarized pump and probe. Spin relaxation time of holes is achieved as a function of excited hole density for the first time at room temperature, and increases with hole density, which disagrees with a theoretical prediction based on EY spin relaxation mechanism, implying that EY mechanism may be not dominant hole spin relaxation mechanism at room temperature, but DP mechanism is dominant possibly.

Ultrafast acousto-optic mode conversion in optically birefringent ferroelectrics

PubMed Central

Lejman, Mariusz; Vaudel, Gwenaelle; Infante, Ingrid C.; Chaban, Ievgeniia; Pezeril, Thomas; Edely, Mathieu; Nataf, Guillaume F.; Guennou, Mael; Kreisel, Jens; Gusev, Vitalyi E.; Dkhil, Brahim; Ruello, Pascal

2016-01-01

The ability to generate efficient giga–terahertz coherent acoustic phonons with femtosecond laser makes acousto-optics a promising candidate for ultrafast light processing, which faces electronic device limits intrinsic to complementary metal oxide semiconductor technology. Modern acousto-optic devices, including optical mode conversion process between ordinary and extraordinary light waves (and vice versa), remain limited to the megahertz range. Here, using coherent acoustic waves generated at tens of gigahertz frequency by a femtosecond laser pulse, we reveal the mode conversion process and show its efficiency in ferroelectric materials such as BiFeO3 and LiNbO3. Further to the experimental evidence, we provide a complete theoretical support to this all-optical ultrafast mechanism mediated by acousto-optic interaction. By allowing the manipulation of light polarization with gigahertz coherent acoustic phonons, our results provide a novel route for the development of next-generation photonic-based devices and highlight new capabilities in using ferroelectrics in modern photonics. PMID:27492493

Large-area tungsten disulfide for ultrafast photonics.

PubMed

Yan, Peiguang; Chen, Hao; Yin, Jinde; Xu, Zihan; Li, Jiarong; Jiang, Zike; Zhang, Wenfei; Wang, Jinzhang; Li, Irene Ling; Sun, Zhipei; Ruan, Shuangchen

2017-02-02

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have attracted significant interest in various optoelectronic applications due to their excellent nonlinear optical properties. One of the most important applications of TMDs is to be employed as an extraordinary optical modulation material (e.g., the saturable absorber (SA)) in ultrafast photonics. The main challenge arises while embedding TMDs into fiber laser systems to generate ultrafast pulse trains and thus constraints their practical applications. Herein, few-layered WS 2 with a large-area was directly transferred on the facet of the pigtail and acted as a SA for erbium-doped fiber laser (EDFL) systems. In our study, WS 2 SA exhibited remarkable nonlinear optical properties (e.g., modulation depth of 15.1% and saturable intensity of 157.6 MW cm -2 ) and was used for ultrafast pulse generation. The soliton pulses with remarkable performances (e.g., ultrashort pulse duration of 1.49 ps, high stability of 71.8 dB, and large pulse average output power of 62.5 mW) could be obtained in a telecommunication band. To the best of our knowledge, the average output power of the mode-locked pulse trains is the highest by employing TMD materials in fiber laser systems. These results indicate that atomically large-area WS 2 could be used as excellent optical modulation materials in ultrafast photonics.

3D microstructuring inside glass by ultrafast laser

NASA Astrophysics Data System (ADS)

Sugioka, Koji; Hanada, Yasutaka; Midorikawa, Katsumi; Kawano, Hiroyuki; Ishikawa, Ikuko S.; Miyawaki, Atsushi

2012-01-01

We demonstrate three-dimensional (3D) microstructuring inside glass by ultrafast laser to fabricate microfluidic chips integrated with some functional microcomponents such as optical attenuators and optical waveguides. The fabricated microchips are applied to understand phenomena and functions of microorganisms and cyanobacteria. Ultrafast laser irradiation followed by thermal treatment and wet etching in dilute hydrofluoric acid solution resulted in fabrication of 3D microfludic structures embedded in a photosensitive glass. The embedded microfludic structures enabled us to easily and efficiently observe Phormidium gliding to the seedling root, which accelerates growth of the vegetable. In addition, integration of optical attenuators and optical waveguides into the microfluidic structures clarified the mechanism of the gliding movement of Phormidium. We termed such integrated microchips nanoaquariums, realizing the highly efficient and functional observation and analysis of various microorganisms.

Ultrafast entanglement of trapped ions

NASA Astrophysics Data System (ADS)

Neyenhuis, Brian; Mizrahi, Jonathan; Johnson, Kale; Monroe, Christopher

2013-05-01

We have demonstrated ultrafast spin-motion entanglement of a single atomic ion using a short train of intense laser pulses. This pulse train gives the ion a spin-dependent kick where each spin state receives a discrete momentum kick in opposite directions. Using a series of these spin-dependent kicks we can realize a two qubit gate. In contrast to gates using spectroscopically resolved motional sidebands, these gates may be performed faster than the trap oscillation period, making them potentially less sensitive to noise, independent of temperature, and more easily scalable to large crystals of ions. We show that multiple kicks can be strung together to create a ``Schrodinger cat'' like state, where the large separation between the two parts of the wavepacket allow us to accumulate the phase shift necessary for a gate in a shorter amount of time. We will present a realistic pulse scheme for a two ion gate, and our progress towards its realization. This work is supported by grants from the U.S. Army Research Office with funding from the DARPA OLE program, IARPA, and the MURI program; and the NSF Physics Frontier Center at JQI.

Optical nonlinearities and ultrafast all-optical switching of m-plane GaN in the near-infrared

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fang, Yu; Zhou, Feng; Yang, Junyi

2015-06-22

We reported a systematic investigation on the three-photon absorption (3PA) spectra and wavelength dispersion of Kerr refraction of bulk m-plane GaN crystal with both polarization E⊥c and E//c by femtosecond Z-scan technique in the near-infrared region from 760 to 1030 nm. Both 3PA spectra and Kerr refraction dispersion were in good agreement with two-band models. The calculated nonlinear figure of merit and measured ultrafast nonlinear refraction dynamics via femtosecond pump-probe with phase object method revealed that m-plane GaN would be a promising candidate for ultrafast all-optical switching and autocorrelation applications at telecommunication wavelengths.

Photon gating in four-dimensional ultrafast electron microscopy.

PubMed

Hassan, Mohammed T; Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H

2015-10-20

Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon-electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a "single" light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a "second" optical pulse has previously been proposed and examined theoretically in our group. Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM.

Photon gating in four-dimensional ultrafast electron microscopy

PubMed Central

Hassan, Mohammed T.; Liu, Haihua; Baskin, John Spencer; Zewail, Ahmed H.

2015-01-01

Ultrafast electron microscopy (UEM) is a pivotal tool for imaging of nanoscale structural dynamics with subparticle resolution on the time scale of atomic motion. Photon-induced near-field electron microscopy (PINEM), a key UEM technique, involves the detection of electrons that have gained energy from a femtosecond optical pulse via photon–electron coupling on nanostructures. PINEM has been applied in various fields of study, from materials science to biological imaging, exploiting the unique spatial, energy, and temporal characteristics of the PINEM electrons gained by interaction with a “single” light pulse. The further potential of photon-gated PINEM electrons in probing ultrafast dynamics of matter and the optical gating of electrons by invoking a “second” optical pulse has previously been proposed and examined theoretically in our group. Here, we experimentally demonstrate this photon-gating technique, and, through diffraction, visualize the phase transition dynamics in vanadium dioxide nanoparticles. With optical gating of PINEM electrons, imaging temporal resolution was improved by a factor of 3 or better, being limited only by the optical pulse widths. This work enables the combination of the high spatial resolution of electron microscopy and the ultrafast temporal response of the optical pulses, which provides a promising approach to attain the resolution of few femtoseconds and attoseconds in UEM. PMID:26438835

Modifying ultrafast optical response of sputtered VOX nanostructures in a broad spectral range by altering post annealing atmosphere

NASA Astrophysics Data System (ADS)

Kürüm, U.; Yaglioglu, H. G.; Küçüköz, B.; Oksuzoglu, R. M.; Yıldırım, M.; Yağcı, A. M.; Yavru, C.; Özgün, S.; Tıraş, T.; Elmali, A.

2015-01-01

Nanostructured VOX thin films were grown in a dc magnetron sputter system under two different Ar:O2 gas flow ratios. The films were annealed under vacuum and various ratios of O2/N2 atmospheres. The insulator-to-metal transition properties of the thin films were investigated by temperature dependent resistance measurement. Photo induced insulator-to-metal transition properties were investigated by Z-scan and ultrafast white light continuum pump probe spectroscopy measurements. Experiments showed that not only insulator-to-metal transition, but also wavelength dependence (from NIR to VIS) and time scale (from ns to ultrafast) of nonlinear optical response of the VOX thin films could be fine tuned by carefully adjusting post annealing atmosphere despite different initial oxygen content in the production. Fabricated VO2 thin films showed reflection change in the visible region due to photo induced phase transition. The results have general implications for easy and more effective fabrication of the nanostructured oxide systems with controllable electrical, optical, and ultrafast optical responses.

Influence of anisotropic dipolar interaction on the spin dynamics of Ni80Fe20 nanodot arrays arranged in honeycomb and octagonal lattices

NASA Astrophysics Data System (ADS)

Mondal, Sucheta; Barman, Saswati; Choudhury, Samiran; Otani, Yoshichika; Barman, Anjan

2018-07-01

Ultrafast spin dynamics in ferromagnetic nanodot arrays with dot diameter 100 nm and thickness 20 nm arranged in honeycomb and octagonal lattice symmetries are studied to explore the tunability of the collective magnetization dynamics. By varying the inter-dot separation between 30 nm and 300 nm drastic variation in the precessional dynamics from strongly collective to completely isolated regime has been observed by using all-optical time-resolved magneto-optical Kerr microscope. Micromagnetic simulation is exploited to gain insights about the resonant mode profiles and magnetic coupling between the nanodots. A significant spectral and spatial variation in the resonant mode with increasing dipolar interaction is demonstrated with increasing inter-dot separation. The spins driven by effective field inside single nanodots are prone to precess independently, generating two self-standing centre and edge modes in the array that are influenced by the relative orientation between the inter-dot coupling direction and bias magnetic field. The anisotropic behavior of dipolar field is rigorously investigated here. Splitting of the centre mode in case of octagonal lattice is experimentally observed here as a consequence of the anisotropic dipolar field between the nanodot pairs coupled horizontally and vertically, which is not found in the honeycomb lattice. In addition, proper understanding of the modification of dynamic mode profile by neighboring dipolar interaction built up here, is imperative for further control of the dynamic dipolar interaction and the corresponding collective excitation in magnonic crystals. The usage of nanodot lattices with complex basis structures can be advantageous for the designing of high density magnetic recording media, spin-wave filter and logic devices.

Direct Characterization of Ultrafast Energy-Time Entangled Photon Pairs.

PubMed

MacLean, Jean-Philippe W; Donohue, John M; Resch, Kevin J

2018-02-02

Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast time scales, making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast time scales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.

Nanoscale solid-state quantum computing

NASA Astrophysics Data System (ADS)

Ardavan, A.; Austwick, M.; Benjamin, S.C.; Briggs, G.A.D.; Dennis, T.J.S.; Ferguson, A.; Hasko, D.G.; Kanai, M.; Khlobystov, A.N.; Lovett, B.W.; Morley, G.W.; Oliver, R.A.; Pettifor, D.G.; Porfyrakis, K.; Reina, J.H.; Rice, J.H.; Smith, J.D.; Taylor, R.A.; Williams, D.A.; Adelmann, C.; Mariette, H.; Hamers, R.J.

2003-07-01

Most experts agree that it is too early to say how quantum computers will eventually be built, and several nanoscale solid-state schemes are being implemented in a range of materials. Nanofabricated quantum dots can be made in designer configurations, with established technology for controlling interactions and for reading out results. Epitaxial quantum dots can be grown in vertical arrays in semiconductors, and ultrafast optical techniques are available for controlling and measuring their excitations. Single-walled carbon nanotubes can be used for molecular self-assembly of endohedral fullerenes, which can embody quantum information in the electron spin. The challenges of individual addressing in such tiny structures could rapidly become intractable with increasing numbers of qubits, but these schemes are amenable to global addressing methods for computation.

Identification of the dominant photochemical pathways and mechanistic insights to the ultrafast ligand exchange of Fe(CO) 5 to Fe(CO) 4EtOH

DOE PAGES

Kunnus, K.; Josefsson, I.; Rajkovic, I.; ...

2016-02-09

We utilized femtosecond time-resolved resonant inelastic X-ray scattering and ab initio theory to study the transient electronic structure and the photoinduced molecular dynamics of a model metal carbonyl photocatalyst Fe(CO) 5 in ethanol solution. We propose mechanistic explanation for the parallel ultrafast intra-molecular spin crossover and ligation of the Fe(CO) 4 which are observed following a charge transfer photoexcitation of Fe(CO) 5 as reported in our previous study [Wernet et al., Nature 520, 78 (2015)]. We find that branching of the reaction pathway likely happens in the 1A 1 state of Fe(CO) 4. A sub-picosecond time constant of themore » spin crossover from 1B 2 to 3B 2 is rationalized by the proposed 1B 2 → 1A 1 → 3B 2 mechanism. Ultrafast ligation of the 1B 2 Fe(CO) 4 state is significantly faster than the spin-forbidden and diffusion limited ligation process occurring from the 3B 2 Fe(CO) 4 ground state that has been observed in the previous studies. We propose that the ultrafast ligation occurs via 1B 2 → 1A 1 → 1A' Fe(CO) 4EtOH pathway and the time scale of the 1A 1 Fe(CO) 4 state ligation is governed by the solute-solvent collision frequency. In conclusion, our study emphasizes the importance of understanding the interaction of molecular excited states with the surrounding environment to explain the relaxation pathways of photoexcited metal carbonyls in solution.« less

The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

ScienceCinema

Mao, Ho-kwang (Director, Center for Energy Frontier Research in Extreme Environments); EFree Staff

2017-12-09

'The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales ' was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Washington and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO{sub 2}, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO{sub 2} (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.

An Ultrafast Switchable Terahertz Polarization Modulator Based on III-V Semiconductor Nanowires.

PubMed

Baig, Sarwat A; Boland, Jessica L; Damry, Djamshid A; Tan, H Hoe; Jagadish, Chennupati; Joyce, Hannah J; Johnston, Michael B

2017-04-12

Progress in the terahertz (THz) region of the electromagnetic spectrum is undergoing major advances, with advanced THz sources and detectors being developed at a rapid pace. Yet, ultrafast THz communication is still to be realized, owing to the lack of practical and effective THz modulators. Here, we present a novel ultrafast active THz polarization modulator based on GaAs semiconductor nanowires arranged in a wire-grid configuration. We utilize an optical pump-terahertz probe spectroscopy system and vary the polarization of the optical pump beam to demonstrate ultrafast THz modulation with a switching time of less than 5 ps and a modulation depth of -8 dB. We achieve an extinction of over 13% and a dynamic range of -9 dB, comparable to microsecond-switchable graphene- and metamaterial-based THz modulators, and surpassing the performance of optically switchable carbon nanotube THz polarizers. We show a broad bandwidth for THz modulation between 0.1 and 4 THz. Thus, this work presents the first THz modulator which combines not only a large modulation depth but also a broad bandwidth and picosecond time resolution for THz intensity and phase modulation, making it an ideal candidate for ultrafast THz communication.

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

PubMed Central

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha; Huber, Bernhard; Bechtel, Hans A.; Sasagawa, Takao; Martin, Michael C.; Lanzara, Alessandra; Kaindl, Robert A.

2017-01-01

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La1.75Sr0.25NiO4, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids. PMID:29202025

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers.

PubMed

Liu, X M; Yang, H R; Cui, Y D; Chen, G W; Yang, Y; Wu, X Q; Yao, X K; Han, D D; Han, X X; Zeng, C; Guo, J; Li, W L; Cheng, G; Tong, L M

2016-05-16

Graphene, whose absorbance is approximately independent of wavelength, allows broadband light-matter interactions with ultrafast responses. The interband optical absorption of graphene can be saturated readily under strong excitation, thereby enabling scientists to exploit the photonic properties of graphene to realize ultrafast lasers. The evanescent field interaction scheme of the propagating light with graphene covered on a D-shaped fibre or microfibre has been employed extensively because of the nonblocking configuration. Obviously, most of the fibre surface is unused in these techniques. Here, we exploit a graphene-clad microfibre (GCM) saturable absorber in a mode-locked fibre laser for the generation of ultrafast pulses. The proposed all-surface technique can guarantee a higher efficiency of light-graphene interactions than the aforementioned techniques. Our GCM-based saturable absorber can generate ultrafast optical pulses within 1.5 μm. This saturable absorber is compatible with current fibre lasers and has many merits such as low saturation intensities, ultrafast recovery times, and wide wavelength ranges. The proposed saturable absorber will pave the way for graphene-based wideband photonics.

Graphene-clad microfibre saturable absorber for ultrafast fibre lasers

PubMed Central

Liu, X. M.; Yang, H. R.; Cui, Y. D.; Chen, G. W.; Yang, Y.; Wu, X. Q.; Yao, X. K.; Han, D. D.; Han, X. X.; Zeng, C.; Guo, J.; Li, W. L.; Cheng, G.; Tong, L. M.

2016-01-01

Graphene, whose absorbance is approximately independent of wavelength, allows broadband light–matter interactions with ultrafast responses. The interband optical absorption of graphene can be saturated readily under strong excitation, thereby enabling scientists to exploit the photonic properties of graphene to realize ultrafast lasers. The evanescent field interaction scheme of the propagating light with graphene covered on a D-shaped fibre or microfibre has been employed extensively because of the nonblocking configuration. Obviously, most of the fibre surface is unused in these techniques. Here, we exploit a graphene-clad microfibre (GCM) saturable absorber in a mode-locked fibre laser for the generation of ultrafast pulses. The proposed all-surface technique can guarantee a higher efficiency of light–graphene interactions than the aforementioned techniques. Our GCM-based saturable absorber can generate ultrafast optical pulses within 1.5 μm. This saturable absorber is compatible with current fibre lasers and has many merits such as low saturation intensities, ultrafast recovery times, and wide wavelength ranges. The proposed saturable absorber will pave the way for graphene-based wideband photonics. PMID:27181419

Testing ultrafast mode-locking at microhertz relative optical linewidth.

PubMed

Martin, Michael J; Foreman, Seth M; Schibli, T R; Ye, Jun

2009-01-19

We report new limits on the phase coherence of the ultrafast mode-locking process in an octave-spanning Ti:sapphire comb.We find that the mode-locking mechanism correlates optical phase across a full optical octave with less than 2.5 microHZ relative linewidth. This result is at least two orders of magnitude below recent predictions for quantum-limited individual comb-mode linewidths, verifying that the mode-locking mechanism strongly correlates quantum noise across the comb spectrum.

Robust tunable excitonic features in monolayer transition metal dichalcogenide quantum dots

NASA Astrophysics Data System (ADS)

Fouladi-Oskouei, J.; Shojaei, S.; Liu, Z.

2018-04-01

The effects of quantum confinement on excitons in parabolic quantum dots of monolayer transition metal dichalcogenides (TMDC QDs) are investigated within a massive Dirac fermion model. A giant spin-valley coupling of the TMDC QDs is obtained, larger than that of monolayer TMDC sheets and consistent with recent experimental measurements. The exciton transition energy and the binding energy are calculated, and it is found that the strong quantum confinement results in extremely high exciton binding energies. The enormously large exciton binding energy in TMDC QDs (({{E}{{B2D}}}∼ 500 meV)<{{E}{{BQD}}}~≲ 1800 meV for different kinds of TMDC QDs) ensures that the many body interactions play a significant role in the investigation of the optical properties of these novel nanostructures. The estimated oscillator strength and radiative lifetime of excitons are strongly size-dependent and indicate a giant oscillator strength enhancement and ultrafast radiative annihilation of excitons, varying from a few tens of femtoseconds to a few picoseconds. We found that the spin-dependent band gap, spin-valley coupling, binding energy and excitonic effects can be tuned by quantum confinements, leading to tunable quantum dots in monolayer TMDCs. This finding offers new functionality in engineering the interaction of a 2D material with light and creates promise for the quantum manipulation of spin and valley degrees of freedom in TMDC nanostructures, enabling versatile novel 2D quantum photonic and optoelectronic nanodevices.

Ultrafast photodissociation dynamics of 1,4-diiodobenzene

NASA Astrophysics Data System (ADS)

Stankus, Brian; Zotev, Nikola; Rogers, David M.; Gao, Yan; Odate, Asami; Kirrander, Adam; Weber, Peter M.

2018-05-01

The photodissociation dynamics of 1,4-diiodobenzene is investigated using ultrafast time-resolved photoelectron spectroscopy. Following excitation by laser pulses at 271 nm, the excited-state dynamics is probed by resonance-enhanced multiphoton ionization with 405 nm probe pulses. A progression of Rydberg states, which come into resonance sequentially, provide a fingerprint of the dissociation dynamics of the molecule. The initial excitation decays with a lifetime of 33 ± 4 fs, in good agreement with a previous study. The spectrum is interpreted by reference to ab initio calculations at the CASPT2(18,14) level, including spin-orbit coupling. We propose that both the 5B1 and 6B1 states are excited initially, and based on the calculations, we identify diabatic spin-orbit coupled states corresponding to the main dissociation pathways.

Characterization of Ultrafast Laser Pulses using a Low-dispersion Frequency Resolved Optical Grating Spectrometer

NASA Astrophysics Data System (ADS)

Whitelock, Hope; Bishop, Michael; Khosravi, Soroush; Obaid, Razib; Berrah, Nora

2016-05-01

A low dispersion frequency-resolved optical gating (FROG) spectrometer was designed to characterize ultrashort (<50 femtosecond) laser pulses from a commercial regenerative amplifier, optical parametric amplifier, and a home-built non-colinear optical parametric amplifier. This instrument splits a laser pulse into two replicas with a 90:10 intensity ratio using a thin pellicle beam-splitter and then recombines the pulses in a birefringent medium. The instrument detects a wavelength-sensitive change in polarization of the weak probe pulse in the presence of the stronger pump pulse inside the birefringent medium. Scanning the time delay between the two pulses and acquiring spectra allows for characterization of the frequency and time content of ultrafast laser pulses, that is needed for interpretation of experimental results obtained from these ultrafast laser systems. Funded by the DoE-BES, Grant No. DE-SC0012376.

Ultrafast saturable absorption in TiS2 induced by non-equilibrium electrons and the generation of a femtosecond mode-locked laser.

PubMed

Tian, Xiangling; Wei, Rongfei; Liu, Meng; Zhu, Chunhui; Luo, Zhichao; Wang, Fengqiu; Qiu, Jianrong

2018-05-24

Non-equilibrium electrons induced by ultrafast laser excitation in a correlated electron material can disturb the Fermi energy as well as optical nonlinearity. Here, non-equilibrium electrons translate a semiconductor TiS2 material into a plasma to generate broad band nonlinear optical saturable absorption with a sub-picosecond recovery time of ∼768 fs (corresponding to modulation frequencies over 1.3 THz) and a modulation response up to ∼145%. Based on this optical nonlinear modulator, a stable femtosecond mode-locked pulse with a pulse duration of ∼402 fs and a pulse train with a period of ∼175.5 ns is observed in the all-optical system. The findings indicate that non-equilibrium electrons can promote a TiS2-based saturable absorber to be an ultrafast switch for a femtosecond pulse output.

Two-Dimensional CH3NH3PbI3 Perovskite Nanosheets for Ultrafast Pulsed Fiber Lasers.

PubMed

Li, Pengfei; Chen, Yao; Yang, Tieshan; Wang, Ziyu; Lin, Han; Xu, Yanhua; Li, Lei; Mu, Haoran; Shivananju, Bannur Nanjunda; Zhang, Yupeng; Zhang, Qinglin; Pan, Anlian; Li, Shaojuan; Tang, Dingyuan; Jia, Baohua; Zhang, Han; Bao, Qiaoliang

2017-04-12

Even though the nonlinear optical effects of solution processed organic-inorganic perovskite films have been studied, the nonlinear optical properties in two-dimensional (2D) perovskites, especially their applications for ultrafast photonics, are largely unexplored. In comparison to bulk perovskite films, 2D perovskite nanosheets with small thicknesses of a few unit cells are more suitable for investigating the intrinsic nonlinear optical properties because bulk recombination of photocarriers and the nonlinear scattering are relatively small. In this research, we systematically investigated the nonlinear optical properties of 2D perovskite nanosheets derived from a combined solution process and vapor phase conversion method. It was found that 2D perovskite nanosheets have stronger saturable absorption properties with large modulation depth and very low saturation intensity compared with those of bulk perovskite films. Using an all dry transfer method, we constructed a new type of saturable absorber device based on single piece 2D perovskite nanosheet. Stable soliton state mode-locking was achieved, and ultrafast picosecond pulses were generated at 1064 nm. This work is likely to pave the way for ultrafast photonic and optoelectronic applications based on 2D perovskites.

Novel optoelectronic devices; Proceedings of the Meeting, The Hague, Netherlands, Mar. 31-Apr. 2, 1987

NASA Technical Reports Server (NTRS)

Adams, Michael J. (Editor)

1987-01-01

The present conference on novel optoelectronics discusses topics in the state-of-the-art in this field in the Netherlands, quantum wells, integrated optics, nonlinear optical devices and fiber-optic-based devices, ultrafast optics, and nonlinear optics and optical bistability. Attention is given to the production of fiber-optics for telecommunications by means of PCVD, lifetime broadening in quantum wells, nonlinear multiple quantum well waveguide devices, tunable single-wavelength lasers, an Si integrated waveguiding polarimeter, and an electrooptic light modulator using long-range surface plasmons. Also discussed are backward-wave couplers and reflectors, a wavelength-selective all-fiber switching matrix, the impact of ultrafast optics in high-speed electronics, the physics of low energy optical switching, and all-optical logical elements for optical processing.

Ultrafast entanglement of trapped ions

NASA Astrophysics Data System (ADS)

Neyenhuis, Brian; Johnson, Kale; Mizrahi, Jonathan; Wong-Campos, David; Monroe, Christopher

2014-05-01

We have demonstrated ultrafast spin-motion entanglement of a single atomic ion using a short train of intense laser pulses. This pulse train gives the ion a spin-dependent kick where each spin state receives a discrete momentum kick in opposite directions. Using a series of these spin-dependent kicks we can realize a two qubit gate. In contrast to gates using spectroscopically resolved motional sidebands, these gates may be performed faster than the trap oscillation period, making them potentially less sensitive to noise. Additionally this gate is temperature insensitive and does not require the ions to be cooled to the Lamb-Dicke limit. We show that multiple kicks can be strung together to create a ``Schrodinger cat'' like state, where the large separation between the two parts of the wavepacket allow us to accumulate the phase shift necessary for a gate in a shorter amount of time. We will present a realistic pulse scheme for a two ion gate, and our progress towards its realization. This work is supported by grants from the U.S. Army Research Office with funding from the DARPA OLE program, IARPA, and the MURI program; and the NSF Physics Frontier Center at JQI.

Optical laser systems at the Linac Coherent Light Source

DOE PAGES

Minitti, Michael P.; Robinson, Joseph S.; Coffee, Ryan N.; ...

2015-04-22

Ultrafast optical lasers play an essential role in exploiting the unique capabilities of recently commissioned X-ray free-electron laser facilities such as the Linac Coherent Light Source (LCLS). Pump–probe experimental techniques reveal ultrafast dynamics in atomic and molecular processes and reveal new insights in chemistry, biology, material science and high-energy-density physics. This manuscript describes the laser systems and experimental methods that enable cutting-edge optical laser/X-ray pump–probe experiments to be performed at LCLS.

Interfacing broadband photonic qubits to on-chip cavity-protected rare-earth ensembles

PubMed Central

Zhong, Tian; Kindem, Jonathan M.; Rochman, Jake; Faraon, Andrei

2017-01-01

Ensembles of solid-state optical emitters enable broadband quantum storage and transduction of photonic qubits, with applications in high-rate quantum networks for secure communications and interconnecting future quantum computers. To transfer quantum states using ensembles, rephasing techniques are used to mitigate fast decoherence resulting from inhomogeneous broadening, but these techniques generally limit the bandwidth, efficiency and active times of the quantum interface. Here, we use a dense ensemble of neodymium rare-earth ions strongly coupled to a nanophotonic resonator to demonstrate a significant cavity protection effect at the single-photon level—a technique to suppress ensemble decoherence due to inhomogeneous broadening. The protected Rabi oscillations between the cavity field and the atomic super-radiant state enable ultra-fast transfer of photonic frequency qubits to the ions (∼50 GHz bandwidth) followed by retrieval with 98.7% fidelity. With the prospect of coupling to other long-lived rare-earth spin states, this technique opens the possibilities for broadband, always-ready quantum memories and fast optical-to-microwave transducers. PMID:28090078

Interfacing broadband photonic qubits to on-chip cavity-protected rare-earth ensembles

NASA Astrophysics Data System (ADS)

Zhong, Tian; Kindem, Jonathan M.; Rochman, Jake; Faraon, Andrei

2017-01-01

Ensembles of solid-state optical emitters enable broadband quantum storage and transduction of photonic qubits, with applications in high-rate quantum networks for secure communications and interconnecting future quantum computers. To transfer quantum states using ensembles, rephasing techniques are used to mitigate fast decoherence resulting from inhomogeneous broadening, but these techniques generally limit the bandwidth, efficiency and active times of the quantum interface. Here, we use a dense ensemble of neodymium rare-earth ions strongly coupled to a nanophotonic resonator to demonstrate a significant cavity protection effect at the single-photon level--a technique to suppress ensemble decoherence due to inhomogeneous broadening. The protected Rabi oscillations between the cavity field and the atomic super-radiant state enable ultra-fast transfer of photonic frequency qubits to the ions (~50 GHz bandwidth) followed by retrieval with 98.7% fidelity. With the prospect of coupling to other long-lived rare-earth spin states, this technique opens the possibilities for broadband, always-ready quantum memories and fast optical-to-microwave transducers.

Advanced optic fabrication using ultrafast laser radiation

NASA Astrophysics Data System (ADS)

Taylor, Lauren L.; Qiao, Jun; Qiao, Jie

2016-03-01

Advanced fabrication and finishing techniques are desired for freeform optics and integrated photonics. Methods including grinding, polishing and magnetorheological finishing used for final figuring and polishing of such optics are time consuming, expensive, and may be unsuitable for complex surface features while common photonics fabrication techniques often limit devices to planar geometries. Laser processing has been investigated as an alternative method for optic forming, surface polishing, structure writing, and welding, as direct tuning of laser parameters and flexible beam delivery are advantageous for complex freeform or photonics elements and material-specific processing. Continuous wave and pulsed laser radiation down to the nanosecond regime have been implemented to achieve nanoscale surface finishes through localized material melting, but the temporal extent of the laser-material interaction often results in the formation of a sub-surface heat affected zone. The temporal brevity of ultrafast laser radiation can allow for the direct vaporization of rough surface asperities with minimal melting, offering the potential for smooth, final surface quality with negligible heat affected material. High intensities achieved in focused ultrafast laser radiation can easily induce phase changes in the bulk of materials for processing applications. We have experimentally tested the effectiveness of ultrafast laser radiation as an alternative laser source for surface processing of monocrystalline silicon. Simulation of material heating associated with ultrafast laser-material interaction has been performed and used to investigate optimized processing parameters including repetition rate. The parameter optimization process and results of experimental processing will be presented.

Charge and spin control of ultrafast electron and hole dynamics in single CdSe/ZnSe quantum dots

NASA Astrophysics Data System (ADS)

Hinz, C.; Gumbsheimer, P.; Traum, C.; Holtkemper, M.; Bauer, B.; Haase, J.; Mahapatra, S.; Frey, A.; Brunner, K.; Reiter, D. E.; Kuhn, T.; Seletskiy, D. V.; Leitenstorfer, A.

2018-01-01

We study the dynamics of photoexcited electrons and holes in single negatively charged CdSe/ZnSe quantum dots with two-color femtosecond pump-probe spectroscopy. An initial characterization of the energy level structure is performed at low temperatures and magnetic fields of up to 5 T. Emission and absorption resonances are assigned to specific transitions between few-fermion states by a theoretical model based on a configuration interaction approach. To analyze the dynamics of individual charge carriers, we initialize the quantum system into excited trion states with defined energy and spin. Subsequently, the time-dependent occupation of the trion ground state is monitored by spectrally resolved differential transmission measurements. We observe subpicosecond dynamics for a hole excited to the D shell. The energy dependence of this D -to-S shell intraband transition is investigated in quantum dots of varying size. Excitation of an electron-hole pair in the respective p shells leads to the formation of singlet and triplet spin configurations. Relaxation of the p -shell singlet is observed to occur on a time scale of a few picoseconds. Pumping of p -shell triplet transitions opens up two pathways with distinctly different scattering times. These processes are shown to be governed by the mixing of singlet and triplet states due to exchange interactions enabling simultaneous electron and hole spin flips. To isolate the relaxation channels, we align the spin of the residual electron by a magnetic field and employ laser pulses of defined helicity. This step provides ultrafast preparation of a fully inverted trion ground state of the quantum dot with near unity probability, enabling deterministic addition of a single photon to the probe pulse. Therefore our experiments represent a significant step towards using single quantum emitters with well-controled inversion to manipulate the photon statistics of ultrafast light pulses.

Ultrafast all-optical imaging technique using low-temperature grown GaAs/AlxGa1 - xAs multiple-quantum-well semiconductor

NASA Astrophysics Data System (ADS)

Gao, Guilong; Tian, Jinshou; Wang, Tao; He, Kai; Zhang, Chunmin; Zhang, Jun; Chen, Shaorong; Jia, Hui; Yuan, Fenfang; Liang, Lingliang; Yan, Xin; Li, Shaohui; Wang, Chao; Yin, Fei

2017-11-01

We report and experimentally demonstrate an ultrafast all-optical imaging technique capable of single-shot ultrafast recording with a picosecond-scale temporal resolution and a micron-order two-dimensional spatial resolution. A GaAs/AlxGa1 - xAs multiple-quantum-well (MQW) semiconductor with a picosecond response time, grown using molecular beam epitaxy (MBE) at a low temperature (LT), is used for the first time in ultrafast imaging technology. The semiconductor transforms the signal beam information to the probe beam, the birefringent delay crystal time-serializes the input probe beam, and the beam displacer maps different polarization probe beams onto different detector locations, resulting in two frames with an approximately 9 ps temporal separation and approximately 25 lp/mm spatial resolution in the visible range.

Double-Wall Carbon Nanotubes for Wide-Band, Ultrafast Pulse Generation

PubMed Central

2014-01-01

We demonstrate wide-band ultrafast optical pulse generation at 1, 1.5, and 2 μm using a single-polymer composite saturable absorber based on double-wall carbon nanotubes (DWNTs). The freestanding optical quality polymer composite is prepared from nanotubes dispersed in water with poly(vinyl alcohol) as the host matrix. The composite is then integrated into ytterbium-, erbium-, and thulium-doped fiber laser cavities. Using this single DWNT–polymer composite, we achieve 4.85 ps, 532 fs, and 1.6 ps mode-locked pulses at 1066, 1559, and 1883 nm, respectively, highlighting the potential of DWNTs for wide-band ultrafast photonics. PMID:24735347

Ultrafast spin dynamics and switching via spin transfer torque in antiferromagnets with weak ferromagnetism

PubMed Central

Kim, Tae Heon; Grünberg, Peter; Han, Song Hee; Cho, Beongki

2016-01-01

The spin-torque driven dynamics of antiferromagnets with Dzyaloshinskii-Moriya interaction (DMI) were investigated based on the Landau-Lifshitz-Gilbert-Slonczewski equation with antiferromagnetic and ferromagnetic order parameters (l and m, respectively). We demonstrate that antiferromagnets including DMI can be described by a 2-dimensional pendulum model of l. Because m is coupled with l, together with DMI and exchange energy, close examination of m provides fundamental understanding of its dynamics in linear and nonlinear regimes. Furthermore, we discuss magnetization reversal as a function of DMI and anisotropy energy induced by a spin current pulse. PMID:27713522

Controlling laser-induced magnetization reversal dynamics in a rare-earth iron garnet across the magnetization compensation point

NASA Astrophysics Data System (ADS)

Deb, Marwan; Molho, Pierre; Barbara, Bernard; Bigot, Jean-Yves

2018-04-01

In this work we explore the ultrafast magnetization dynamics induced by femtosecond laser pulses in a doped film of gadolinium iron garnet over a broad temperature range including the magnetization compensation point TM. By exciting the phonon-assisted 6S→4G and 6S→4P electronic d -d transitions simultaneously by one- and two-photon absorption processes, we find out that the transfer of heat energy from the lattice to the spin has, at a temperature slightly below TM, a large influence on the magnetization dynamics. In particular, we show that the speed and the amplitude of the magnetization dynamics can be strongly increased when increasing either the external magnetic field or the laser energy density. The obtained results are explained by a magnetization reversal process across TM. Furthermore, we find that the dynamics has unusual characteristics which can be understood by considering the weak spin-phonon coupling in magnetic garnets. These results open new perspectives for controlling the magnetic state of magnetic dielectrics using an ultrashort optically induced heat pulse.

A hybrid quantum eraser scheme for characterization of free-space and fiber communication channels

NASA Astrophysics Data System (ADS)

Nape, Isaac; Kyeremah, Charlotte; Vallés, Adam; Rosales-Guzmán, Carmelo; Buah-Bassuah, Paul K.; Forbes, Andrew

2018-02-01

We demonstrate a simple projective measurement based on the quantum eraser concept that can be used to characterize the disturbances of any communication channel. Quantum erasers are commonly implemented as spatially separated path interferometric schemes. Here we exploit the advantages of redefining the which-path information in terms of spatial modes, replacing physical paths with abstract paths of orbital angular momentum (OAM). Remarkably, vector modes (natural modes of free-space and fiber) have a non-separable feature of spin-orbit coupled states, equivalent to the description of two independently marked paths. We explore the effects of fiber perturbations by probing a step-index optical fiber channel with a vector mode, relevant to high-order spatial mode encoding of information for ultra-fast fiber communications.

Ultrafast Laser Beam Switching and Pulse Train Generation by Using Coupled Vertical-Cavity, Surface-Emitting Lasers (VCSELS)

NASA Technical Reports Server (NTRS)

Goorjian, Peter M. (Inventor); Ning, Cun-Zheng (Inventor)

2005-01-01

Ultrafast directional beam switching is achieved using coupled VCSELs. This approach is demonstrated to achieve beam switching frequencies of 40 GHz and more and switching directions of about eight degrees. This switching scheme is likely to be useful for ultrafast optical networks at frequencies much higher than achievable with other approaches.

Ultrafast Graphene Light Emitters.

PubMed

Kim, Young Duck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Bae, Myung-Ho; Kim, Hyungsik; Seo, Dongjea; Choi, Heon-Jin; Kim, Suk Hyun; Nemilentsau, Andrei; Low, Tony; Tan, Cheng; Efetov, Dmitri K; Taniguchi, Takashi; Watanabe, Kenji; Shepard, Kenneth L; Heinz, Tony F; Englund, Dirk; Hone, James

2018-02-14

Ultrafast electrically driven nanoscale light sources are critical components in nanophotonics. Compound semiconductor-based light sources for the nanophotonic platforms have been extensively investigated over the past decades. However, monolithic ultrafast light sources with a small footprint remain a challenge. Here, we demonstrate electrically driven ultrafast graphene light emitters that achieve light pulse generation with up to 10 GHz bandwidth across a broad spectral range from the visible to the near-infrared. The fast response results from ultrafast charge-carrier dynamics in graphene and weak electron-acoustic phonon-mediated coupling between the electronic and lattice degrees of freedom. We also find that encapsulating graphene with hexagonal boron nitride (hBN) layers strongly modifies the emission spectrum by changing the local optical density of states, thus providing up to 460% enhancement compared to the gray-body thermal radiation for a broad peak centered at 720 nm. Furthermore, the hBN encapsulation layers permit stable and bright visible thermal radiation with electronic temperatures up to 2000 K under ambient conditions as well as efficient ultrafast electronic cooling via near-field coupling to hybrid polaritonic modes under electrical excitation. These high-speed graphene light emitters provide a promising path for on-chip light sources for optical communications and other optoelectronic applications.

Supercomputations and big-data analysis in strong-field ultrafast optical physics: filamentation of high-peak-power ultrashort laser pulses

NASA Astrophysics Data System (ADS)

Voronin, A. A.; Panchenko, V. Ya; Zheltikov, A. M.

2016-06-01

High-intensity ultrashort laser pulses propagating in gas media or in condensed matter undergo complex nonlinear spatiotemporal evolution where temporal transformations of optical field waveforms are strongly coupled to an intricate beam dynamics and ultrafast field-induced ionization processes. At the level of laser peak powers orders of magnitude above the critical power of self-focusing, the beam exhibits modulation instabilities, producing random field hot spots and breaking up into multiple noise-seeded filaments. This problem is described by a (3  +  1)-dimensional nonlinear field evolution equation, which needs to be solved jointly with the equation for ultrafast ionization of a medium. Analysis of this problem, which is equivalent to solving a billion-dimensional evolution problem, is only possible by means of supercomputer simulations augmented with coordinated big-data processing of large volumes of information acquired through theory-guiding experiments and supercomputations. Here, we review the main challenges of supercomputations and big-data processing encountered in strong-field ultrafast optical physics and discuss strategies to confront these challenges.

Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces

DOE PAGES

Shcherbakov, Maxim R.; Liu, Sheng; Zubyuk, Varvara V.; ...

2017-05-12

Optical metasurfaces are regular quasi-planar nanopatterns that can apply diverse spatial and spectral transformations to light waves. But, metasurfaces are no longer adjustable after fabrication, and a critical challenge is to realise a technique of tuning their optical properties that is both fast and efficient. Here, we experimentally realise an ultrafast tunable metasurface consisting of subwavelength gallium arsenide nanoparticles supporting Mie-type resonances in the near infrared. In using transient reflectance spectroscopy, we demonstrate a picosecond-scale absolute reflectance modulation of up to 0.35 at the magnetic dipole resonance of the metasurfaces and a spectral shift of the resonance by 30 nm,more » both achieved at unprecedentedly low pump fluences of less than 400 μJ cm –2. Our findings thereby enable a versatile tool for ultrafast and efficient control of light using light.« less

Ultrafast all-optical tuning of direct-gap semiconductor metasurfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shcherbakov, Maxim R.; Liu, Sheng; Zubyuk, Varvara V.

Optical metasurfaces are regular quasi-planar nanopatterns that can apply diverse spatial and spectral transformations to light waves. But, metasurfaces are no longer adjustable after fabrication, and a critical challenge is to realise a technique of tuning their optical properties that is both fast and efficient. Here, we experimentally realise an ultrafast tunable metasurface consisting of subwavelength gallium arsenide nanoparticles supporting Mie-type resonances in the near infrared. In using transient reflectance spectroscopy, we demonstrate a picosecond-scale absolute reflectance modulation of up to 0.35 at the magnetic dipole resonance of the metasurfaces and a spectral shift of the resonance by 30 nm,more » both achieved at unprecedentedly low pump fluences of less than 400 μJ cm –2. Our findings thereby enable a versatile tool for ultrafast and efficient control of light using light.« less

Broadband nonlinear optical response of monolayer MoSe2 under ultrafast excitation

NASA Astrophysics Data System (ADS)

Nie, Zhonghui; Trovatello, Chiara; Pogna, Eva A. A.; Dal Conte, Stefano; Miranda, Paulo B.; Kelleher, Edmund; Zhu, Chunhui; Turcu, Ion Crisitan Edmond; Xu, Yongbing; Liu, Kaihui; Cerullo, Giulio; Wang, Fengqiu

2018-01-01

Due to their strong light-matter interaction, monolayer transition metal dichalcogenides (TMDs) have proven to be promising candidates for nonlinear optics and optoelectronics. Here, we characterize the nonlinear absorption of chemical vapour deposition (CVD)-grown monolayer MoSe2 in the 720-810 nm wavelength range. Surprisingly, despite the presence of strong exciton resonances, monolayer MoSe2 exhibits a uniform modulation depth of ˜80 ± 3% and a saturation intensity of ˜2.5 ± 0.4 MW/cm2. In addition, pump-probe spectroscopy is performed to confirm the saturable absorption and reveal the photocarrier relaxation dynamics over hundreds of picoseconds. Our results unravel the unique broadband nonlinear absorptive behavior of monolayer MoSe2 under ultrafast excitation and highlight the potential of using monolayer TMDs as broadband ultrafast optical switches with customizable saturable absorption characteristics.

The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A "Life at the Frontiers of Energy Research" contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

DOE Office of Scientific and Technical Information (OSTI.GOV)

None

"The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales" was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the "Life at the Frontiers of Energy Research" video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Science in Washington, DC and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office ofmore » Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO2, water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO2 (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.« less

Light-induced pyroelectric effect as an effective approach for ultrafast ultraviolet nanosensing

NASA Astrophysics Data System (ADS)

Wang, Zhaona; Yu, Ruomeng; Pan, Caofeng; Li, Zhaoling; Yang, Jin; Yi, Fang; Wang, Zhong Lin

2015-09-01

Zinc oxide is potentially a useful material for ultraviolet detectors; however, a relatively long response time hinders practical implementation. Here by designing and fabricating a self-powered ZnO/perovskite-heterostructured ultraviolet photodetector, the pyroelectric effect, induced in wurtzite ZnO nanowires on ultraviolet illumination, has been utilized as an effective approach for high-performance photon sensing. The response time is improved from 5.4 s to 53 μs at the rising edge, and 8.9 s to 63 μs at the falling edge, with an enhancement of five orders in magnitudes. The specific detectivity and the responsivity are both enhanced by 322%. This work provides a novel design to achieve ultrafast ultraviolet sensing at room temperature via light-self-induced pyroelectric effect. The newly designed ultrafast self-powered ultraviolet nanosensors may find promising applications in ultrafast optics, nonlinear optics, optothermal detections, computational memories and biocompatible optoelectronic probes.

Layer-Dependent Ultrafast Carrier and Coherent Phonon Dynamics in Black Phosphorus.

PubMed

Miao, Xianchong; Zhang, Guowei; Wang, Fanjie; Yan, Hugen; Ji, Minbiao

2018-05-09

Black phosphorus is a layered semiconducting material, demonstrating strong layer-dependent optical and electronic properties. Probing the photophysical properties on ultrafast time scales is of central importance in understanding many-body interactions and nonequilibrium quasiparticle dynamics. Here, we applied temporally, spectrally, and spatially resolved pump-probe microscopy to study the transient optical responses of mechanically exfoliated few-layer black phosphorus, with layer numbers ranging from 2 to 9. We have observed layer-dependent resonant transient absorption spectra with both photobleaching and red-shifted photoinduced absorption features, which could be attributed to band gap renormalization of higher subband transitions. Surprisingly, coherent phonon oscillations with unprecedented intensities were observed when the probe photons were in resonance with the optical transitions, which correspond to the low-frequency layer-breathing mode. Our results reveal strong Coulomb interactions and electron-phonon couplings in photoexcited black phosphorus, providing important insights into the ultrafast optical, nanomechanical, and optoelectronic properties of this novel two-dimensional material.

Design of high-efficiency diffractive optical elements towards ultrafast mid-infrared time-stretched imaging and spectroscopy

NASA Astrophysics Data System (ADS)

Xie, Hongbo; Ren, Delun; Wang, Chao; Mao, Chensheng; Yang, Lei

2018-02-01

Ultrafast time stretch imaging offers unprecedented imaging speed and enables new discoveries in scientific research and engineering. One challenge in exploiting time stretch imaging in mid-infrared is the lack of high-quality diffractive optical elements (DOEs), which encode the image information into mid-infrared optical spectrum. This work reports the design and optimization of mid-infrared DOE with high diffraction-efficiency, broad bandwidth and large field of view. Using various typical materials with their refractive indices ranging from 1.32 to 4.06 in ? mid-infrared band, diffraction efficiencies of single-layer and double-layer DOEs have been studied in different wavelength bands with different field of views. More importantly, by replacing the air gap of double-layer DOE with carefully selected optical materials, one optimized ? triple-layer DOE, with efficiency higher than 95% in the whole ? mid-infrared window and field of view greater than ?, is designed and analyzed. This new DOE device holds great potential in ultrafast mid-infrared time stretch imaging and spectroscopy.

Measurement of ultrafast optical Kerr effect of Ge-Sb-Se chalcogenide slab waveguides by the beam self-trapping technique

NASA Astrophysics Data System (ADS)

Kuriakose, Tintu; Baudet, Emeline; Halenkovič, Tomáš; Elsawy, Mahmoud M. R.; Němec, Petr; Nazabal, Virginie; Renversez, Gilles; Chauvet, Mathieu

2017-11-01

We present a reliable and original experimental technique based on the analysis of beam self-trapping to measure ultrafast optical nonlinearities in planar waveguides. The technique is applied to the characterization of Ge-Sb-Se chalcogenide films that allow Kerr induced self-focusing and soliton formation. Linear and nonlinear optical constants of three different chalcogenide waveguides are studied at 1200 and 1550 nm in femtosecond regime. Waveguide propagation loss and two photon absorption coefficients are determined by transmission analysis. Beam broadening and narrowing results are compared with simulations of the nonlinear Schrödinger equation solved by BPM method to deduce the Kerr n2 coefficients. Kerr optical nonlinearities obtained by our original technique compare favorably with the values obtained by Z-scan technique. Nonlinear refractive index as high as (69 ± 11) × 10-18m2 / W is measured in Ge12.5Sb25Se62.5 at 1200 nm with low nonlinear absorption and low propagation losses which reveals the great characteristics of our waveguides for ultrafast all optical switching and integrated photonic devices.

Long-period fiber gratings as ultrafast optical differentiators.

PubMed

Kulishov, Mykola; Azaña, José

2005-10-15

It is demonstrated that a single, uniform long-period fiber grating (LPFG) working in the linear regime inherently behaves as an ultrafast optical temporal differentiator. Specifically, we show that the output temporal waveform in the core mode of a LPFG providing full energy coupling into the cladding mode is proportional to the first derivative of the optical temporal signal (e.g., optical pulse) launched at the input of the LPFG. Moreover, a LPFG providing full energy recoupling back from the cladding mode into the core mode inherently implements second-order temporal differentiation. Our numerical results have confirmed the feasibility of this simple, all-fiber approach to processing optical signals with temporal features in the picosecond and subpicosecond ranges.

Ultra-fast all-optical plasmonic switching in near infra-red spectrum using a Kerr nonlinear ring resonator

NASA Astrophysics Data System (ADS)

Nurmohammadi, Tofiq; Abbasian, Karim; Yadipour, Reza

2018-03-01

In this paper, an all-optical plasmonic switch based on metal-insulator-metal (MIM) nanoplasmonic waveguide with a Kerr nonlinear ring resonator is introduced and studied. Two-dimensional simulations utilizing the finite-difference time-domain algorithm are used to demonstrate an apparent optical bistability and significant switching mechanisms (in enabled-low condition: T(ON/OFF) =21.9 and in enabled-high condition: T(ON/OFF) =24.9) of the signal light arisen by altering the pump-light intensity. The proposed all-optical switching demonstrates femtosecond-scale feedback time (90 fs) and then ultra-fast switching can be achieved. The offered all-optical switch may recognize potential significant applications in integrated optical circuits.

Proton-detected 3D {sup 1}H/{sup 13}C/{sup 1}H correlation experiment for structural analysis in rigid solids under ultrafast-MAS above 60 kHz

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Rongchun; Ramamoorthy, Ayyalusamy, E-mail: ramamoor@umich.edu; Nishiyama, Yusuke

2015-10-28

A proton-detected 3D {sup 1}H/{sup 13}C/{sup 1}H chemical shift correlation experiment is proposed for the assignment of chemical shift resonances, identification of {sup 13}C-{sup 1}H connectivities, and proximities of {sup 13}C-{sup 1}H and {sup 1}H-{sup 1}H nuclei under ultrafast magic-angle-spinning (ultrafast-MAS) conditions. Ultrafast-MAS is used to suppress all anisotropic interactions including {sup 1}H-{sup 1}H dipolar couplings, while the finite-pulse radio frequency driven dipolar recoupling (fp-RFDR) pulse sequence is used to recouple dipolar couplings among protons and the insensitive nuclei enhanced by polarization transfer technique is used to transfer magnetization between heteronuclear spins. The 3D experiment eliminates signals from non-carbon-bonded protonsmore » and non-proton-bonded carbons to enhance spectral resolution. The 2D (F1/F3) {sup 1}H/{sup 1}H and 2D {sup 13}C/{sup 1}H (F2/F3) chemical shift correlation spectra extracted from the 3D spectrum enable the identification of {sup 1}H-{sup 1}H proximity and {sup 13}C-{sup 1}H connectivity. In addition, the 2D (F1/F2) {sup 1}H/{sup 13}C chemical shift correlation spectrum, incorporated with proton magnetization exchange via the fp-RFDR recoupling of {sup 1}H-{sup 1}H dipolar couplings, enables the measurement of proximities between {sup 13}C and even the remote non-carbon-bonded protons. The 3D experiment also gives three-spin proximities of {sup 1}H-{sup 1}H-{sup 13}C chains. Experimental results obtained from powder samples of L-alanine and L-histidine ⋅ H{sub 2}O ⋅ HCl demonstrate the efficiency of the 3D experiment.« less

Ultrafast MR imaging of the pelvic floor.

PubMed

Unterweger, M; Marincek, B; Gottstein-Aalame, N; Debatin, J F; Seifert, B; Ochsenbein-Imhof, N; Perucchini, D; Kubik-Huch, R A

2001-04-01

The aim of this study was to compare pelvic floor anatomy and laxity at rest and on straining (Valsalva's maneuver) using dynamic ultrafast MR imaging in women who were continent versus those with stress incontinence differing in obstetric history. Thirty continent women were divided into three equal groups (nulliparous, previous cesarean delivery, previous vaginal delivery) and compared with 10 women with stress-incontinence with a history of at least one vaginal delivery. MR imaging of the pelvic floor at rest and on maximal strain was performed, using axial T2-weighted fast spin-echo images followed by sagittal ultrafast T2-weighted single-shot fast spin-echo sequences. Mean population age (age range, 22-45 years; mean +/- SD, 36 +/- 5.4 years), was similar in the four groups, as was parity in the three parous groups. Mean distances between the bladder floor and pubococcygeal line at rest did not differ between the four groups. On straining, bladder floor descent was 1.1 +/- 0.9, 1.0 +/- 1.1, and 1.9 +/- 0.9 cm in continent nulliparous, cesarean delivery, and vaginal delivery women, respectively, versus 3.2 +/- 1.0 cm in incontinent women (p = 0.0005). Cervical descent was greater in incontinent versus nulliparous women (p = 0.0019). Bladder floor descent was greater in the continent vaginal delivery group than in continent cesarean delivery control patients (p = 0.04). In patients with stress incontinence, symptoms did not correlate with amplitude of descent. The right levator muscle was thinner overall than the left, regardless of frequency direction (p = 0.001). Ultrafast MR imaging using the T2-weighted single-shot fast spin-echo sequence allows dynamic evaluation of the pelvic compartments at maximal strain with no need for contrast medium. Pelvic floor laxity and supporting fascia abnormalities were most common in patients with stress incontinence followed by continent women with a history of vaginal delivery. The results are therefore compatible with the hypothesis of vaginal delivery as a contributory factor to stress incontinence in older parous women.

Photoinduced surface plasmon switching at VO2/Au interface.

PubMed

Kumar, Nardeep; Rúa, Armando; Aldama, Jennifer; Echeverría, Karla; Fernández, Félix E; Lysenko, Sergiy

2018-05-28

Angle-resolved reflection, light scattering and ultrafast pump-probe spectroscopy combined with a surface plasmon-polariton (SPP) resonance technique in attenuated total reflection geometry was used to investigate the light-induced plasmonic switching in a photorefractive VO 2 /Au hybrid structure. Measurements of SPP scattering and reflection shows that the optically-induced formation of metallic state in a vanadium dioxide layer deposited on a gold film significantly alters the electromagnetic field enhancement and SPP propagation length at the VO 2 /Au interface. The ultrafast optical manipulation of SPP resonance is shown on a picosecond timescale. Obtained results demonstrate high potential of photorefractive vanadium oxides as efficient plasmonic modulating materials for ultrafast optoelectronic devices.

Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency.

PubMed

Li, Chi; Zhou, Xu; Zhai, Feng; Li, Zhenjun; Yao, Fengrui; Qiao, Ruixi; Chen, Ke; Cole, Matthew Thomas; Yu, Dapeng; Sun, Zhipei; Liu, Kaihui; Dai, Qing

2017-08-01

Ultrafast electron pulses, combined with laser-pump and electron-probe technologies, allow ultrafast dynamics to be characterized in materials. However, the pursuit of simultaneous ultimate spatial and temporal resolution of microscopy and spectroscopy is largely subdued by the low monochromaticity of the electron pulses and their poor phase synchronization to the optical excitation pulses. Field-driven photoemission from metal tips provides high light-phase synchronization, but suffers large electron energy spreads (3-100 eV) as driven by a long wavelength laser (>800 nm). Here, ultrafast electron emission from carbon nanotubes (≈1 nm radius) excited by a 410 nm femtosecond laser is realized in the field-driven regime. In addition, the emitted electrons have great monochromaticity with energy spread as low as 0.25 eV. This great performance benefits from the extraordinarily high field enhancement and great stability of carbon nanotubes, superior to metal tips. The new nanotube-based ultrafast electron source opens exciting prospects for extending current characterization to sub-femtosecond temporal resolution as well as sub-nanometer spatial resolution. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast all-optical technologies for bidirectional optical wireless communications.

PubMed

Jin, Xian; Hristovski, Blago A; Collier, Christopher M; Geoffroy-Gagnon, Simon; Born, Brandon; Holzman, Jonathan F

2015-04-01

In this Letter, a spherical retro-modulator architecture is introduced for operation as a bidirectional transceiver in passive optical wireless communication links. The architecture uses spherical retroreflection to enable retroreflection with broad directionality (2π steradians), and it uses all-optical beam interaction to enable modulation on ultrafast timescales (120 fs duration). The spherical retro-modulator is investigated from a theoretical standpoint and is fabricated for testing with three glasses, N-BK7, N-LASF9, and S-LAH79. It is found that the S-LAH79 structure provides the optimal refraction and nonlinearity for the desired retroreflection and modulation capabilities.

Femtosecond laser spectroscopy of the rhodopsin photochromic reaction: a concept for ultrafast optical molecular switch creation (ultrafast reversible photoreaction of rhodopsin).

PubMed

Smitienko, Olga; Nadtochenko, Victor; Feldman, Tatiana; Balatskaya, Maria; Shelaev, Ivan; Gostev, Fedor; Sarkisov, Oleg; Ostrovsky, Mikhail

2014-11-11

Ultrafast reverse photoreaction of visual pigment rhodopsin in the femtosecond time range at room temperature is demonstrated. Femtosecond two-pump probe experiments with a time resolution of 25 fs have been performed. The first рump pulse at 500 nm initiated cis-trans photoisomerization of rhodopsin chromophore, 11-cis retinal, which resulted in the formation of the primary ground-state photoproduct within a mere 200 fs. The second pump pulse at 620 nm with a varying delay of 200 to 3750 fs relative to the first рump pulse, initiated the reverse phototransition of the primary photoproduct to rhodopsin. The results of this photoconversion have been observed on the differential spectra obtained after the action of two pump pulses at a time delay of 100 ps. It was found that optical density decreased at 560 nm in the spectral region of bathorhodopsin absorption and increased at 480 nm, where rhodopsin absorbs. Rhodopsin photoswitching efficiency shows oscillations as a function of the time delay between two рump pulses. The quantum yield of reverse photoreaction initiated by the second pump pulse falls within the range 15%±1%. The molecular mechanism of the ultrafast reversible photoreaction of visual pigment rhodopsin may be used as a concept for the development of an ultrafast optical molecular switch.

Ultrafast Non-thermal Response of Plasmonic Resonance in Gold Nanoantennas

NASA Astrophysics Data System (ADS)

Soavi, Giancarlo; Valle, Giuseppe Della; Biagioni, Paolo; Cattoni, Andrea; Longhi, Stefano; Cerullo, Giulio; Brida, Daniele

Ultrafast thermalization of electrons in metal nanostructures is studied by means of pump-probe spectroscopy. We track in real-time the plasmon resonance evolution, providing a tool for understanding and controlling gold nanoantennas non-linear optical response.

Ultrafast time-resolved photoemission of a metallic tip/substrate junction

NASA Astrophysics Data System (ADS)

Meng, Xiang; Jin, Wencan; Yang, Hao; Dadap, Jerry; Osgood, Richard; Camillone, Nicholas, III

The strong near-field enhancement of metallic-tip nanostructures has attracted great interest in scanning microscopy techniques, such as surface-enhanced Raman scattering, near-field scanning optical microscopy and tip-enhanced nonlinear imaging. In this talk, we use a full vectorial 3D-FDTD method to investigate the spatial characteristics of the optical field confinement and localization between a tungsten nanoprobe and an infinite planar silver substrate, with two-color ultrafast laser excitation scheme. The degree of two-color excited field enhancement, geometry dependence, the exact mechanism of optical tip-substrate coupling and tip-substrate plasmon resonances are significant in understanding the electrodynamical responses at tip-substrate junction. The demonstrated measurements with subpicosecond time and subnanometer spatial resolution suggest a new approach to ultrafast time-resolved measurements of surface electron dynamics. DE-FG 02-90-ER-14104; DE-FG 02-04-ER-46157.

Ultrafast optical ranging using microresonator soliton frequency combs

NASA Astrophysics Data System (ADS)

Trocha, P.; Karpov, M.; Ganin, D.; Pfeiffer, M. H. P.; Kordts, A.; Wolf, S.; Krockenberger, J.; Marin-Palomo, P.; Weimann, C.; Randel, S.; Freude, W.; Kippenberg, T. J.; Koos, C.

2018-02-01

Light detection and ranging is widely used in science and industry. Over the past decade, optical frequency combs were shown to offer advantages in optical ranging, enabling fast distance acquisition with high accuracy. Driven by emerging high-volume applications such as industrial sensing, drone navigation, or autonomous driving, there is now a growing demand for compact ranging systems. Here, we show that soliton Kerr comb generation in integrated silicon nitride microresonators provides a route to high-performance chip-scale ranging systems. We demonstrate dual-comb distance measurements with Allan deviations down to 12 nanometers at averaging times of 13 microseconds along with ultrafast ranging at acquisition rates of 100 megahertz, allowing for in-flight sampling of gun projectiles moving at 150 meters per second. Combining integrated soliton-comb ranging systems with chip-scale nanophotonic phased arrays could enable compact ultrafast ranging systems for emerging mass applications.

Ultrafast nonlinear optical properties of thin-solid DNA film and their application as a saturable absorber in femtosecond mode-locked fiber laser

PubMed Central

Khazaeinezhad, Reza; Hosseinzadeh Kassani, Sahar; Paulson, Bjorn; Jeong, Hwanseong; Gwak, Jiyoon; Rotermund, Fabian; Yeom, Dong-Il; Oh, Kyunghwan

2017-01-01

A new extraordinary application of deoxyribonucleic acid (DNA) thin-solid-film was experimentally explored in the field of ultrafast nonlinear photonics. Optical transmission was investigated in both linear and nonlinear regimes for two types of DNA thin-solid-films made from DNA in aqueous solution and DNA-cetyltrimethylammonium chloride (CTMA) in an organic solvent. Z-scan measurements revealed a high third-order nonlinearity with n2 exceeding 10−9 at a wavelength of 1570 nm, for a nonlinarity about five orders of magnitude larger than that of silica. We also demonstrated ultrafast saturable absorption (SA) with a modulation depth of 0.43%. DNA thin solid films were successfully deposited on a side-polished optical fiber, providing an efficient evanescent wave interaction. We built an organic-inorganic hybrid all-fiber ring laser using DNA film as an ultrafast SA and using Erbium-doped fiber as an efficient optical gain medium. Stable transform-limited femtosecond soliton pulses were generated with full width half maxima of 417 fs for DNA and 323 fs for DNA-CTMA thin-solid-film SAs. The average output power was 4.20 mW for DNA and 5.46 mW for DNA-CTMA. Detailed conditions for DNA solid film preparation, dispersion control in the laser cavity and subsequent characteristics of soliton pulses are discussed, to confirm unique nonlinear optical applications of DNA thin-solid-film. PMID:28128340

Spatially and temporally resolved exciton dynamics and transport in single nanostructures and assemblies

NASA Astrophysics Data System (ADS)

Huang, Libai

2015-03-01

The frontier in solar energy conversion now lies in learning how to integrate functional entities across multiple length scales to create optimal devices. To address this new frontier, I will discuss our recent efforts on elucidating multi-scale energy transfer, migration, and dissipation processes with simultaneous femtosecond temporal resolution and nanometer spatial resolution. We have developed ultrafast microscopy that combines ultrafast spectroscopy with optical microscopy to map exciton dynamics and transport with simultaneous ultrafast time resolution and diffraction-limited spatial resolution. We have employed pump-probe transient absorption microscopy to elucidate morphology and structure dependent exciton dynamics and transport in single nanostructures and molecular assemblies. More specifically, (1) We have applied transient absorption microscopy (TAM) to probe environmental and structure dependent exciton relaxation pathways in sing-walled carbon nanotubes (SWNTs) by mapping dynamics in individual pristine SWNTs with known structures. (2) We have systematically measured and modeled the optical properties of the Frenkel excitons in self-assembled porphyrin tubular aggregates that represent an analog to natural photosynthetic antennae. Using a combination of ultrafast optical microscopy and stochastic exciton modeling, we address exciton transport and relaxation pathways, especially those related to disorder.

Ultrafast optics. Ultrafast optical control by few photons in engineered fiber.

PubMed

Nissim, R; Pejkic, A; Myslivets, E; Kuo, B P; Alic, N; Radic, S

2014-07-25

Fast control of a strong optical beam by a few photons is an outstanding challenge that limits the performance of quantum sensors and optical processing devices. We report that a fast and efficient optical gate can be realized in an optical fiber that has been engineered with molecular-scale accuracy. Highly efficient, distributed phase-matched photon-photon interaction was achieved in the fiber with locally controlled, nanometer-scale core variations. A three-photon input was used to manipulate a Watt-scale beam at a speed exceeding 500 gigahertz. In addition to very fast beam control, the results provide a path to developing a new class of sensitive receivers capable of operating at very high rates. Copyright © 2014, American Association for the Advancement of Science.

Ultrafast transient grating radiation to optical image converter

DOEpatents

Stewart, Richard E; Vernon, Stephen P; Steel, Paul T; Lowry, Mark E

2014-11-04

A high sensitivity transient grating ultrafast radiation to optical image converter is based on a fixed transmission grating adjacent to a semiconductor substrate. X-rays or optical radiation passing through the fixed transmission grating is thereby modulated and produces a small periodic variation of refractive index or transient grating in the semiconductor through carrier induced refractive index shifts. An optical or infrared probe beam tuned just below the semiconductor band gap is reflected off a high reflectivity mirror on the semiconductor so that it double passes therethrough and interacts with the radiation induced phase grating therein. A small portion of the optical beam is diffracted out of the probe beam by the radiation induced transient grating to become the converted signal that is imaged onto a detector.

Quantum and semiclassical physics behind ultrafast optical nonlinearity in the midinfrared: the role of ionization dynamics within the field half cycle.

PubMed

Serebryannikov, E E; Zheltikov, A M

2014-07-25

Ultrafast ionization dynamics within the field half cycle is shown to be the key physical factor that controls the properties of optical nonlinearity as a function of the carrier wavelength and intensity of a driving laser field. The Schrödinger-equation analysis of a generic hydrogen quantum system reveals universal tendencies in the wavelength dependence of optical nonlinearity, shedding light on unusual properties of optical nonlinearities in the midinfrared. For high-intensity low-frequency fields, free-state electrons are shown to dominate over bound electrons in the overall nonlinear response of a quantum system. In this regime, semiclassical models are shown to offer useful insights into the physics behind optical nonlinearity.

Nonlinear-optical activity owing to anisotropy of ultrafast nonlinear refraction in cubic materials.

PubMed

Hutchings, D C

1995-08-01

The evolution of the polarization state in a cubic material with an anisotropic Kerr nonlinearity is examined. It is shown that in certain cases this provides a mechanism for nonlinear-optical activity, leaving the state of the polarization unchanged but causing a signif icant rotation in its major axis. The use of the anisotropic ultrafast nonlinear refraction that exists just beneath the half-gap in semiconductors to demonstrate these effects is discussed.

Ultrafast Graphene Photonics and Optoelectronics

DTIC Science & Technology

2017-04-14

SUBJECT TERMS Graphene, Ultrafast Optical Processin, Terahertz Electronics ; 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT SAR 18...Rep, (2016)) Fig. 4. (a) Images of scanning electron microscope for 1D and 2D gratings. (b) Ratio of the real part of the transmitted field

Enhanced Ultrafast Nonlinear Optics With Microstructure Fibers And Photonic Crystals

DTIC Science & Technology

2004-07-01

NANOHOLES FREQUENCY-TUNABLE ANTI-STOKES LINE EMISSION BY EIGENMODES OF A BIREFRINGENT MICROSTRUCTURE FIBER GENERATION OF FEMTOSECOND ANTI-STOKES PULSES...laser technologies, and ultrafast photonics. ANTI-STOKES GENERATION IN GUIDED MODES OF PHOTONIC-CRYSTAL FIBERS MODIFIED WITH AN ARRAY OF NANOHOLES

Shaping ultrafast laser inscribed optical waveguides using a deformable mirror.

PubMed

Thomson, R R; Bockelt, A S; Ramsay, E; Beecher, S; Greenaway, A H; Kar, A K; Reid, D T

2008-08-18

We use a two-dimensional deformable mirror to shape the spatial profile of an ultrafast laser beam that is then used to inscribe structures in a soda-lime silica glass slide. By doing so we demonstrate that it is possible to control the asymmetry of the cross section of ultrafast laser inscribed optical waveguides via the curvature of the deformable mirror. When tested using 1.55 mum light, the optimum waveguide exhibited coupling losses of approximately 0.2 dB/facet to Corning SMF-28 single mode fiber and propagation losses of approximately 1.5 dB.cm(-1). This technique promises the possibility of combining rapid processing speeds with the ability to vary the waveguide cross section along its length.

Coherent Amplification of Ultrafast Molecular Dynamics in an Optical Oscillator

NASA Astrophysics Data System (ADS)

Aharonovich, Igal; Pe'er, Avi

2016-02-01

Optical oscillators present a powerful optimization mechanism. The inherent competition for the gain resources between possible modes of oscillation entails the prevalence of the most efficient single mode. We harness this "ultrafast" coherent feedback to optimize an optical field in time, and show that, when an optical oscillator based on a molecular gain medium is synchronously pumped by ultrashort pulses, a temporally coherent multimode field can develop that optimally dumps a general, dynamically evolving vibrational wave packet, into a single vibrational target state. Measuring the emitted field opens a new window to visualization and control of fast molecular dynamics. The realization of such a coherent oscillator with hot alkali dimers appears within experimental reach.

Staggered Multiple-PRF Ultrafast Color Doppler.

PubMed

Posada, Daniel; Poree, Jonathan; Pellissier, Arnaud; Chayer, Boris; Tournoux, Francois; Cloutier, Guy; Garcia, Damien

2016-06-01

Color Doppler imaging is an established pulsed ultrasound technique to visualize blood flow non-invasively. High-frame-rate (ultrafast) color Doppler, by emissions of plane or circular wavefronts, allows severalfold increase in frame rates. Conventional and ultrafast color Doppler are both limited by the range-velocity dilemma, which may result in velocity folding (aliasing) for large depths and/or large velocities. We investigated multiple pulse-repetition-frequency (PRF) emissions arranged in a series of staggered intervals to remove aliasing in ultrafast color Doppler. Staggered PRF is an emission process where time delays between successive pulse transmissions change in an alternating way. We tested staggered dual- and triple-PRF ultrafast color Doppler, 1) in vitro in a spinning disc and a free jet flow, and 2) in vivo in a human left ventricle. The in vitro results showed that the Nyquist velocity could be extended to up to 6 times the conventional limit. We found coefficients of determination r(2) ≥ 0.98 between the de-aliased and ground-truth velocities. Consistent de-aliased Doppler images were also obtained in the human left heart. Our results demonstrate that staggered multiple-PRF ultrafast color Doppler is efficient for high-velocity high-frame-rate blood flow imaging. This is particularly relevant for new developments in ultrasound imaging relying on accurate velocity measurements.

System and method for ultrafast optical signal detecting via a synchronously coupled anamorphic light pulse encoded laterally

DOEpatents

Heebner, John E [Livermore, CA

2010-08-03

In one general embodiment, a method for ultrafast optical signal detecting is provided. In operation, a first optical input signal is propagated through a first wave guiding layer of a waveguide. Additionally, a second optical input signal is propagated through a second wave guiding layer of the waveguide. Furthermore, an optical control signal is applied to a top of the waveguide, the optical control signal being oriented diagonally relative to the top of the waveguide such that the application is used to influence at least a portion of the first optical input signal propagating through the first wave guiding layer of the waveguide. In addition, the first and the second optical input signals output from the waveguide are combined. Further, the combined optical signals output from the waveguide are detected. In another general embodiment, a system for ultrafast optical signal recording is provided comprising a waveguide including a plurality of wave guiding layers, an optical control source positioned to propagate an optical control signal towards the waveguide in a diagonal orientation relative to a top of the waveguide, at least one optical input source positioned to input an optical input signal into at least a first and a second wave guiding layer of the waveguide, and a detector for detecting at least one interference pattern output from the waveguide, where at least one of the interference patterns results from a combination of the optical input signals input into the first and the second wave guiding layer. Furthermore, propagation of the optical control signal is used to influence at least a portion of the optical input signal propagating through the first wave guiding layer of the waveguide.

Coherent ultrafast spin-dynamics probed in three dimensional topological insulators

PubMed Central

Boschini, F.; Mansurova, M.; Mussler, G.; Kampmeier, J.; Grützmacher, D.; Braun, L.; Katmis, F.; Moodera, J. S.; Dallera, C.; Carpene, E.; Franz, C.; Czerner, M.; Heiliger, C.; Kampfrath, T.; Münzenberg, M.

2015-01-01

Topological insulators are candidates to open up a novel route in spin based electronics. Different to traditional ferromagnetic materials, where the carrier spin-polarization and magnetization are based on the exchange interaction, the spin properties in topological insulators are based on the coupling of spin- and orbit interaction connected to its momentum. Specific ways to control the spin-polarization with light have been demonstrated: the energy momentum landscape of the Dirac cone provides spin-momentum locking of the charge current and its spin. We investigate a spin-related signal present only during the laser excitation studying real and imaginary part of the complex Kerr angle by disentangling spin and lattice contributions. This coherent signal is only present at the time of the pump-pulses’ light field and can be described in terms of a Raman coherence time. The Raman transition involves states at the bottom edge of the conduction band. We demonstrate a coherent femtosecond control of spin-polarization for electronic states at around the Dirac cone. PMID:26510509

Ultrafast optical excitations in supramolecular metallacycles with charge transfer properties.

PubMed

Flynn, Daniel C; Ramakrishna, Guda; Yang, Hai-Bo; Northrop, Brian H; Stang, Peter J; Goodson, Theodore

2010-02-03

New organometallic materials such as two-dimensional metallacycles and three-dimensional metallacages are important for the development of novel optical, electronic, and energy related applications. In this article, the ultrafast dynamics of two different platinum-containing metallacycles have been investigated by femtosecond fluorescence upconversion and transient absorption. These measurements were carried out in an effort to probe the charge transfer dynamics and the rate of intersystem crossing in metallacycles of different geometries and dimensions. The processes of ultrafast intersystem crossing and charge transfer vary between the two different classes of metallacyclic systems studied. For rectangular anthracene-containing metallacycles, the electronic coupling between adjacent ligands was relatively weak, whereas for the triangular phenanthrene-containing structures, there was a clear interaction between the conjugated ligand and the metal complex center. The transient lifetimes increased with increasing conjugation in that case. The results show that differences in the dimensionality and structure of metallacycles result in different optical properties, which may be utilized in the design of nonlinear optical materials and potential new, longer-lived excited state materials for further electronic applications.

Optical detection of three modes of endocytosis at hippocampal synapses

PubMed Central

Chanaday, Natali L

2018-01-01

Coupling of synaptic vesicle fusion and retrieval constitutes a core mechanism ensuring maintenance of presynaptic function. Recent studies using fast-freeze electron microscopy and capacitance measurements reported an ultrafast mode of endocytosis operating at physiological temperatures. Here, using rat hippocampal neurons, we optically monitored single synaptic vesicle endocytosis with high time resolution using the vesicular glutamate transporter, synaptophysin and the V0a1 subunit of the vacuolar ATPase as probes. In this setting, we could distinguish three components of retrieval operating at ultrafast (~150–250 ms, ~20% of events), fast (~5–12 s, ~40% of events) and ultraslow speeds (>20 s, ~40% of events). While increasing Ca2+ slowed the fast events, increasing temperature accelerated their time course. In contrast, the kinetics of ultrafast events were only mildly affected by these manipulations. These results suggest that synaptic vesicle proteins can be retrieved with ultrafast kinetics, although a majority of evoked fusion events are coupled to slower retrieval mechanisms. PMID:29683423

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

NASA Astrophysics Data System (ADS)

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-10-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions

PubMed Central

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A.; Holleitner, Alexander W.

2016-01-01

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches. PMID:27762291

THz-circuits driven by photo-thermoelectric, gate-tunable graphene-junctions.

PubMed

Brenneis, Andreas; Schade, Felix; Drieschner, Simon; Heimbach, Florian; Karl, Helmut; Garrido, Jose A; Holleitner, Alexander W

2016-10-20

For future on-chip communication schemes, it is essential to integrate nanoscale materials with an ultrafast optoelectronic functionality into high-frequency circuits. The atomically thin graphene has been widely demonstrated to be suitable for photovoltaic and optoelectronic devices because of its broadband optical absorption and its high electron mobility. Moreover, the ultrafast relaxation of photogenerated charge carriers has been verified in graphene. Here, we show that dual-gated graphene junctions can be functional parts of THz-circuits. As the underlying optoelectronic process, we exploit ultrafast photo-thermoelectric currents. We describe an immediate photo-thermoelectric current of the unbiased device following a femtosecond laser excitation. For a picosecond time-scale after the optical excitation, an additional photo-thermoelectric contribution shows up, which exhibits the fingerprint of a spatially inverted temperature profile. The latter can be understood by the different time-constants and thermal coupling mechanisms of the electron and phonon baths within graphene to the substrate and the metal contacts. The interplay of the processes gives rise to ultrafast electromagnetic transients in high-frequency circuits, and it is equally important for a fundamental understanding of graphene-based ultrafast photodetectors and switches.

Emerging Low-Dimensional Materials for Nonlinear Optics and Ultrafast Photonics.

PubMed

Liu, Xiaofeng; Guo, Qiangbing; Qiu, Jianrong

2017-04-01

Low-dimensional (LD) materials demonstrate intriguing optical properties, which lead to applications in diverse fields, such as photonics, biomedicine and energy. Due to modulation of electronic structure by the reduced structural dimensionality, LD versions of metal, semiconductor and topological insulators (TIs) at the same time bear distinct nonlinear optical (NLO) properties as compared with their bulk counterparts. Their interaction with short pulse laser excitation exhibits a strong nonlinear character manifested by NLO absorption, giving rise to optical limiting or saturated absorption associated with excited state absorption and Pauli blocking in different materials. In particular, the saturable absorption of these emerging LD materials including two-dimensional semiconductors as well as colloidal TI nanoparticles has recently been utilized for Q-switching and mode-locking ultra-short pulse generation across the visible, near infrared and middle infrared wavelength regions. Beside the large operation bandwidth, these ultrafast photonics applications are especially benefit from the high recovery rate as well as the facile processibility of these LD materials. The prominent NLO response of these LD materials have also provided new avenues for the development of novel NLO and photonics devices for all-optical control as well as optical circuits beyond ultrafast lasers. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrafast monoenergetic electron source by optical waveform control of surface plasmons.

PubMed

Dombi, Péter; Rácz, Péter

2008-03-03

We propose coherent control of photoelectron acceleration at metal surfaces mediated by surface plasmon polaritons. A high degree of spectral and spatial control of the emission process can be exercised by amplitude and phase controlling the optical waveform (including the carrier-envelope phase) of the plasmon generating few-cycle laser pulse. Numerical results show that the emitted electron beam is highly directional and monoenergetic suggesting applications in contemporary ultrafast methods where ultrashort, well-behaved electron pulses are required.

Directly probing spin dynamics in insulating antiferromagnets using ultrashort terahertz pulses

DOE PAGES

Bowlan, Pamela Renee; Trugman, Stuart Alan; Wang, X.; ...

2016-11-22

We investigate spin dynamics in the antiferromagnetic (AFM) multiferroic TbMnO3 using opticalpump, terahertz (THz)-probe spectroscopy. Photoexcitation results in a broadband THz transmission change, with an onset time of 25 ps at 6 K that becomes faster at higher temperatures. We attribute this time constant to spin-lattice thermalization. The excellent agreement between our measurements and previous ultrafast resonant x-ray diffraction measurements on the same material confirms that our THz pulse directly probes spin order. We suggest that this could be the case in general for insulating AFM materials, if the origin of the static absorption in the THz spectral range ismore » magnetic.« less

Influence of optical pumping wavelength on the ultrafast gain and phase recovery acceleration of quantum-dot semiconductor optical amplifiers

NASA Astrophysics Data System (ADS)

Kim, Jungho

2013-10-01

We numerically investigate the influence of the optical pumping wavelength on the ultrafast gain and phase recovery acceleration of quantum-dot (QD) semiconductor optical amplifiers (SOAs) by solving 1088 coupled rate equations. The temporal variations of the gain and phase recovery response at the ground state (GS) of QDs are calculated at various signal wavelengths when the optical pumping wavelengths at the excited state (ES) of QDs are varied. The phase recovery response is fastest when the wavelength of the signal and pumping beams corresponds to the respective emission wavelength of the GS and the ES in the same size of QDs. The absorption efficiency of the optical pumping beam at the ES is determined by the Lorentzian line shape function of the homogeneous broadening.

Magneto-Plasmonics and Resonant Interaction of Light with Dynamic Magnetisation in Metallic and All-Magneto-Dielectric Nanostructures

PubMed Central

Maksymov, Ivan S.

2015-01-01

A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two different points of view: magneto-plasmonics, and magnonics and magnetisation dynamics. It is expected that this presentation style will make this review paper of particular interest to both general physical audience and specialists conducting research on photonics, plasmonics, Brillouin light scattering spectroscopy of magnetic nanostructures and magneto-optical Kerr effect magnetometry, as well as ultrafast all-optical and THz-wave excitation of spin waves. Moreover, readers interested in a new, rapidly emerging field of all-dielectric nanophotonics will find a section about all-magneto-dielectric nanostructures. PMID:28347027

Magneto-Plasmonics and Resonant Interaction of Light with Dynamic Magnetisation in Metallic and All-Magneto-Dielectric Nanostructures.

PubMed

Maksymov, Ivan S

2015-04-09

A significant interest in combining plasmonics and magnetism at the nanoscale gains momentum in both photonics and magnetism sectors that are concerned with the resonant enhancement of light-magnetic-matter interaction in nanostructures. These efforts result in a considerable amount of literature, which is difficult to collect and digest in limited time. Furthermore, there is insufficient exchange of results between the two research sectors. Consequently, the goal of this review paper is to bridge this gap by presenting an overview of recent progress in the field of magneto-plasmonics from two different points of view: magneto-plasmonics, and magnonics and magnetisation dynamics. It is expected that this presentation style will make this review paper of particular interest to both general physical audience and specialists conducting research on photonics, plasmonics, Brillouin light scattering spectroscopy of magnetic nanostructures and magneto-optical Kerr effect magnetometry, as well as ultrafast all-optical and THz-wave excitation of spin waves. Moreover, readers interested in a new, rapidly emerging field of all-dielectric nanophotonics will find a section about all-magneto-dielectric nanostructures.

Lightwave-driven quasiparticle collisions on a subcycle timescale

NASA Astrophysics Data System (ADS)

Langer, F.; Hohenleutner, M.; Schmid, C. P.; Poellmann, C.; Nagler, P.; Korn, T.; Schüller, C.; Sherwin, M. S.; Huttner, U.; Steiner, J. T.; Koch, S. W.; Kira, M.; Huber, R.

2016-05-01

Ever since Ernest Rutherford scattered α-particles from gold foils, collision experiments have revealed insights into atoms, nuclei and elementary particles. In solids, many-body correlations lead to characteristic resonances—called quasiparticles—such as excitons, dropletons, polarons and Cooper pairs. The structure and dynamics of quasiparticles are important because they define macroscopic phenomena such as Mott insulating states, spontaneous spin- and charge-order, and high-temperature superconductivity. However, the extremely short lifetimes of these entities make practical implementations of a suitable collider challenging. Here we exploit lightwave-driven charge transport, the foundation of attosecond science, to explore ultrafast quasiparticle collisions directly in the time domain: a femtosecond optical pulse creates excitonic electron-hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying dynamics of the wave packets, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands of the optical excitation. A full quantum theory explains our observations microscopically. This approach enables collision experiments with various complex quasiparticles and suggests a promising new way of generating sub-femtosecond pulses.

Lightwave-driven quasiparticle collisions on a subcycle timescale.

PubMed

Langer, F; Hohenleutner, M; Schmid, C P; Poellmann, C; Nagler, P; Korn, T; Schüller, C; Sherwin, M S; Huttner, U; Steiner, J T; Koch, S W; Kira, M; Huber, R

2016-05-12

Ever since Ernest Rutherford scattered α-particles from gold foils, collision experiments have revealed insights into atoms, nuclei and elementary particles. In solids, many-body correlations lead to characteristic resonances--called quasiparticles--such as excitons, dropletons, polarons and Cooper pairs. The structure and dynamics of quasiparticles are important because they define macroscopic phenomena such as Mott insulating states, spontaneous spin- and charge-order, and high-temperature superconductivity. However, the extremely short lifetimes of these entities make practical implementations of a suitable collider challenging. Here we exploit lightwave-driven charge transport, the foundation of attosecond science, to explore ultrafast quasiparticle collisions directly in the time domain: a femtosecond optical pulse creates excitonic electron-hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying dynamics of the wave packets, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands of the optical excitation. A full quantum theory explains our observations microscopically. This approach enables collision experiments with various complex quasiparticles and suggests a promising new way of generating sub-femtosecond pulses.

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

NASA Astrophysics Data System (ADS)

Kono, Junichiro

2013-02-01

Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the Journal of Physics: Condensed Matter staff for their help, patience and professionalism. Since this is a fast-moving field, there is absolutely no way of presenting definitive answers to all open questions, but we hope that this special section will provide an overview of the current state of knowledge regarding this topic. Furthermore, we hope that the exciting science and technology described in this section will attract and inspire other researchers and students working in related fields to enter into the study of ultrafast and nonlinear optical phenomena in carbon-based nanostructures. Ultrafast and nonlinear optics in carbon nanomaterials contents Ultrafast and nonlinear optics in carbon nanomaterialsJunichiro Kono The impact of pump fluence on carrier relaxation dynamics in optically excited grapheneT Winzer and E Malic Time-resolved spectroscopy on epitaxial graphene in the infrared spectral range: relaxation dynamics and saturation behaviorS Winnerl, F Göttfert, M Mittendorff, H Schneider, M Helm, T Winzer, E Malic, A Knorr, M Orlita, M Potemski, M Sprinkle, C Berger and W A de Heer Nonlinear optics of graphene in a strong magnetic fieldXianghan Yao and Alexey Belyanin Theory of coherent phonons in carbon nanotubes and graphene nanoribbonsG D Sanders, A R T Nugraha, K Sato, J-H Kim3, J Kono3, R Saito and C J Stanton Non-perturbative effects of laser illumination on the electrical properties of graphene nanoribbons Hernán L Calvo, Pablo M Perez-Piskunow, Horacio M Pastawski, Stephan Roche and Luis E F Foa Torres Transient absorption microscopy studies of energy relaxation in graphene oxide thin film Sean Murphy and Libai Huang Femtosecond dynamics of exciton localization: self-trapping from the small to the large polaron limit F X Morrissey, J G Mance, A D Van Pelt and S L Dexheimer

Effects of iron on the lattice thermal conductivity of Earth's deep mantle and implications for mantle dynamics

NASA Astrophysics Data System (ADS)

Hsieh, Wen-Pin; Deschamps, Frédéric; Okuchi, Takuo; Lin, Jung-Fu

2018-04-01

Iron may critically influence the physical properties and thermochemical structures of Earth's lower mantle. Its effects on thermal conductivity, with possible consequences on heat transfer and mantle dynamics, however, remain largely unknown. We measured the lattice thermal conductivity of lower-mantle ferropericlase to 120 GPa using the ultrafast optical pump-probe technique in a diamond anvil cell. The thermal conductivity of ferropericlase with 56% iron significantly drops by a factor of 1.8 across the spin transition around 53 GPa, while that with 8–10% iron increases monotonically with pressure, causing an enhanced iron substitution effect in the low-spin state. Combined with bridgmanite data, modeling of our results provides a self-consistent radial profile of lower-mantle thermal conductivity, which is dominated by pressure, temperature, and iron effects, and shows a twofold increase from top to bottom of the lower mantle. Such increase in thermal conductivity may delay the cooling of the core, while its decrease with iron content may enhance the dynamics of large low shear-wave velocity provinces. Our findings further show that, if hot and strongly enriched in iron, the seismic ultralow velocity zones have exceptionally low conductivity, thus delaying their cooling.

Effects of iron on the lattice thermal conductivity of Earth's deep mantle and implications for mantle dynamics.

PubMed

Hsieh, Wen-Pin; Deschamps, Frédéric; Okuchi, Takuo; Lin, Jung-Fu

2018-04-17

Iron may critically influence the physical properties and thermochemical structures of Earth's lower mantle. Its effects on thermal conductivity, with possible consequences on heat transfer and mantle dynamics, however, remain largely unknown. We measured the lattice thermal conductivity of lower-mantle ferropericlase to 120 GPa using the ultrafast optical pump-probe technique in a diamond anvil cell. The thermal conductivity of ferropericlase with 56% iron significantly drops by a factor of 1.8 across the spin transition around 53 GPa, while that with 8-10% iron increases monotonically with pressure, causing an enhanced iron substitution effect in the low-spin state. Combined with bridgmanite data, modeling of our results provides a self-consistent radial profile of lower-mantle thermal conductivity, which is dominated by pressure, temperature, and iron effects, and shows a twofold increase from top to bottom of the lower mantle. Such increase in thermal conductivity may delay the cooling of the core, while its decrease with iron content may enhance the dynamics of large low shear-wave velocity provinces. Our findings further show that, if hot and strongly enriched in iron, the seismic ultralow velocity zones have exceptionally low conductivity, thus delaying their cooling.

Optical nonlinearities in plasmonic metamaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Zayats, Anatoly V.

2016-04-01

Metals exhibit strong and fast nonlinearities making metallic, plasmonic, structures very promising for ultrafast all-optical applications at low light intensities. Combining metallic nanostructures in metamaterials provides additional functionalities via prospect of precise engineering of spectral response and dispersion. From this point of view, hyperbolic metamaterials, in particular those based on plasmonic nanorod arrays, provide wealth of exciting possibilities in nonlinear optics offering designed linear and nonlinear properties, polarization control, spontaneous emission control and many others. Experiments and modeling have already demonstrated very strong Kerr-nonlinear response and its ultrafast recovery due to the nonlocal nature of the plasmonic mode of the metamaterial, so that small changes in the permittivity of the metallic component under the excitation modify the nonlocal response that in turn leads to strong changes of the metamaterial transmission. In this talk, we will discuss experimental studies and numerical modeling of second- and third-order nonlinear optical processes in hyperbolic metamaterials based on metallic nanorods and other plasmonic systems where coupling between the resonances plays important role in defining nonlinear response. Second-harmonic generation and ultrafast Kerr-type nonlinearity originating from metallic component of the metamaterial will be considered, including nonlinear magneto-optical effects. Nonlinear optical response of stand-alone as well as integrated metamaterial components will be presented. Some of the examples to be discussed include nonlinear polarization control, nonlinear metamaterial integrated in silicon photonic circuitry and second-harmonic generation, including magneto-optical effects.

Single-shot Monitoring of Ultrafast Processes via X-ray Streaking at a Free Electron Laser.

PubMed

Buzzi, Michele; Makita, Mikako; Howald, Ludovic; Kleibert, Armin; Vodungbo, Boris; Maldonado, Pablo; Raabe, Jörg; Jaouen, Nicolas; Redlin, Harald; Tiedtke, Kai; Oppeneer, Peter M; David, Christian; Nolting, Frithjof; Lüning, Jan

2017-08-03

The advent of x-ray free electron lasers has extended the unique capabilities of resonant x-ray spectroscopy techniques to ultrafast time scales. Here, we report on a novel experimental method that allows retrieving with a single x-ray pulse the time evolution of an ultrafast process, not only at a few discrete time delays, but continuously over an extended time window. We used a single x-ray pulse to resolve the laser-induced ultrafast demagnetisation dynamics in a thin cobalt film over a time window of about 1.6 ps with an excellent signal to noise ratio. From one representative single shot measurement we extract a spin relaxation time of (130 ± 30) fs with an average value, based on 193 single shot events of (113 ± 20) fs. These results are limited by the achieved experimental time resolution of 120 fs, and both values are in excellent agreement with previous results and theoretical modelling. More generally, this new experimental approach to ultrafast x-ray spectroscopy paves the way to the study of non-repetitive processes that cannot be investigated using traditional repetitive pump-probe schemes.

Real-Time Observation of Internal Motion within Ultrafast Dissipative Optical Soliton Molecules

NASA Astrophysics Data System (ADS)

Krupa, Katarzyna; Nithyanandan, K.; Andral, Ugo; Tchofo-Dinda, Patrice; Grelu, Philippe

2017-06-01

Real-time access to the internal ultrafast dynamics of complex dissipative optical systems opens new explorations of pulse-pulse interactions and dynamic patterns. We present the first direct experimental evidence of the internal motion of a dissipative optical soliton molecule generated in a passively mode-locked erbium-doped fiber laser. We map the internal motion of a soliton pair molecule by using a dispersive Fourier-transform imaging technique, revealing different categories of internal pulsations, including vibrationlike and phase drifting dynamics. Our experiments agree well with numerical predictions and bring insights to the analogy between self-organized states of lights and states of the matter.

Mitigating intrinsic defects and laser damage using pulsetrain-burst (>100 MHz) ultrafast laser processing

NASA Astrophysics Data System (ADS)

McKinney, Luke; Frank, Felix; Graper, David; Dean, Jesse; Forrester, Paul; Rioblanc, Maxence; Nantel, Marc; Marjoribanks, Robin

2005-09-01

Ultrafast-laser micromachining has promise as an approach to trimming and 'healing' small laser-produced damage sites in laser-system optics--a common experience in state-of-the-art high-power laser systems. More-conventional approaches currently include mechanical micromachining, chemical modification, and treatment using cw and long-pulse lasers. Laser-optics materials of interest include fused silica, multilayer dielectric stacks for anti-reflection coatings or high-reflectivity mirrors, and inorganic crystals such as KD*P, used for Pockels cells and frequency-doubling. We report on novel efforts using ultrafast-laser pulsetrain-burst processing (microsecond bursts at 133 MHz) to mitigate damage in fused silica, dielectric coatings, and KD*P crystals. We have established the characteristics of pulsetrain-burst micromachining in fused silica, multilayer mirrors, and KD*P, and determined the etch rates and morphology under different conditions of fluence-delivery. From all of these, we have begun to identify new means to optimize the laser-repair of optics defects and damage.

Electron and lattice dynamics of transition metal thin films observed by ultrafast electron diffraction and transient optical measurements.

PubMed

Nakamura, A; Shimojima, T; Nakano, M; Iwasa, Y; Ishizaka, K

2016-11-01

We report the ultrafast dynamics of electrons and lattice in transition metal thin films (Au, Cu, and Mo) investigated by a combination of ultrafast electron diffraction (UED) and pump-probe optical methods. For a single-crystalline Au thin film, we observe the suppression of the diffraction intensity occuring in 10 ps, which direcly reflects the lattice thermalization via the electron-phonon interaction. By using the two-temperature model, the electron-phonon coupling constant ( g ) and the electron and lattice temperatures ( T e , T l ) are evaluated from UED, with which we simulate the transient optical transmittance. The simulation well agrees with the experimentally obtained transmittance data, except for the slight deviations at the initial photoexcitation and the relaxed quasi-equilibrium state. We also present the results similarly obtained for polycrystalline Au, Cu, and Mo thin films and demonstrate the electron and lattice dynamics occurring in metals with different electron-phonon coupling strengths.

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions.

PubMed

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-20

Pulsed lasers operating in the mid-infrared (3-20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd 3 As 2 , a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd 3 As 2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources.

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions

PubMed Central

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-01

Pulsed lasers operating in the mid-infrared (3–20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd3As2, a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd3As2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources. PMID:28106037

A robust and tuneable mid-infrared optical switch enabled by bulk Dirac fermions

NASA Astrophysics Data System (ADS)

Zhu, Chunhui; Wang, Fengqiu; Meng, Yafei; Yuan, Xiang; Xiu, Faxian; Luo, Hongyu; Wang, Yazhou; Li, Jianfeng; Lv, Xinjie; He, Liang; Xu, Yongbing; Liu, Junfeng; Zhang, Chao; Shi, Yi; Zhang, Rong; Zhu, Shining

2017-01-01

Pulsed lasers operating in the mid-infrared (3-20 μm) are important for a wide range of applications in sensing, spectroscopy, imaging and communications. Despite recent advances with mid-infrared gain platforms, the lack of a capable pulse generation mechanism remains a significant technological challenge. Here we show that bulk Dirac fermions in molecular beam epitaxy grown crystalline Cd3As2, a three-dimensional topological Dirac semimetal, constitutes an exceptional ultrafast optical switching mechanism for the mid-infrared. Significantly, we show robust and effective tuning of the scattering channels of Dirac fermions via an element doping approach, where photocarrier relaxation times are found flexibly controlled over an order of magnitude (from 8 ps to 800 fs at 4.5 μm). Our findings reveal the strong impact of Cr doping on ultrafast optical properties in Cd3As2 and open up the long sought parameter space crucial for the development of compact and high-performance mid-infrared ultrafast sources.

Laser-induced spin protection and switching in a specially designed magnetic dot: A theoretical investigation

NASA Astrophysics Data System (ADS)

Zhang, G. P.; Si, M. S.; George, T. F.

2011-04-01

Most laser-induced femtosecond magnetism investigations are done in magnetic thin films. Nanostructured magnetic dots, with their reduced dimensionality, present new opportunities for spin manipulation. Here we predict that if a magnetic dot has a dipole-forbidden transition between the lowest occupied molecular orbital (LUMO) and the highest unoccupied molecular orbital (HOMO), but a dipole-allowed transition between LUMO+1 and HOMO, electromagnetically induced transparency can be used to prevent ultrafast laser-induced spin momentum reduction, or spin protection. This is realized through a strong dump pulse to funnel the population into LUMO+1. If the time delay between the pump and dump pulses is longer than 60 fs, a population inversion starts and spin switching is achieved. These predictions are detectable experimentally.

Satellite transitions acquired in real time by magic angle spinning (STARTMAS): ``Ultrafast'' high-resolution MAS NMR spectroscopy of spin I =3/2 nuclei

NASA Astrophysics Data System (ADS)

Thrippleton, Michael J.; Ball, Thomas J.; Wimperis, Stephen

2008-01-01

The satellite transitions acquired in real time by magic angle spinning (STARTMAS) NMR experiment combines a train of pulses with sample rotation at the magic angle to refocus the first- and second-order quadrupolar broadening of spin I =3/2 nuclei in a series of echoes, while allowing the isotropic chemical and quadrupolar shifts to evolve. The result is real-time isotropic NMR spectra at high spinning rates using conventional MAS equipment. In this paper we describe in detail how STARTMAS data can be acquired and processed with ease on commercial equipment. We also discuss the advantages and limitations of the approach and illustrate the discussion with numerical simulations and experimental data from four different powdered solids.

Quantum simulation of ultrafast dynamics using trapped ultracold atoms.

PubMed

Senaratne, Ruwan; Rajagopal, Shankari V; Shimasaki, Toshihiko; Dotti, Peter E; Fujiwara, Kurt M; Singh, Kevin; Geiger, Zachary A; Weld, David M

2018-05-25

Ultrafast electronic dynamics are typically studied using pulsed lasers. Here we demonstrate a complementary experimental approach: quantum simulation of ultrafast dynamics using trapped ultracold atoms. Counter-intuitively, this technique emulates some of the fastest processes in atomic physics with some of the slowest, leading to a temporal magnification factor of up to 12 orders of magnitude. In these experiments, time-varying forces on neutral atoms in the ground state of a tunable optical trap emulate the electric fields of a pulsed laser acting on bound charged particles. We demonstrate the correspondence with ultrafast science by a sequence of experiments: nonlinear spectroscopy of a many-body bound state, control of the excitation spectrum by potential shaping, observation of sub-cycle unbinding dynamics during strong few-cycle pulses, and direct measurement of carrier-envelope phase dependence of the response to an ultrafast-equivalent pulse. These results establish cold-atom quantum simulation as a complementary tool for studying ultrafast dynamics.

H.sub.2O doped WO.sub.3, ultra-fast, high-sensitivity hydrogen sensors

DOEpatents

Liu, Ping [Denver, CO; Tracy, C Edwin [Golden, CO; Pitts, J Roland [Lakewood, CO; Lee, Se-Hee [Lakewood, CO

2011-03-22

An ultra-fast response, high sensitivity structure for optical detection of low concentrations of hydrogen gas, comprising: a substrate; a water-doped WO.sub.3 layer coated on the substrate; and a palladium layer coated on the water-doped WO.sub.3 layer.

Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics

NASA Astrophysics Data System (ADS)

Wang, Huihui; Bokarev, Sergey I.; Aziz, Saadullah G.; Kühn, Oliver

2017-08-01

Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic timescales. Spin-flip dynamics is usually considered in the context of valence electronic states, where spin-orbit coupling is weak and processes related to the electron spin are usually driven by nuclear motion. However, for core-excited states, where the core-hole has a nonzero angular momentum, spin-orbit coupling is strong enough to drive spin-flips on a much shorter timescale. Using density matrix-based time-dependent restricted active space configuration interaction including spin-orbit coupling, we address an unprecedentedly short spin-crossover for the example of L-edge (2p→3d) excited states of a prototypical Fe(II) complex. This process occurs on a timescale, which is faster than that of Auger decay (∼4 fs) treated here explicitly. Modest variations of carrier frequency and pulse duration can lead to substantial changes in the spin-state yield, suggesting its control by soft X-ray light.

Modern applications of terahertz emission spectroscopy

NASA Astrophysics Data System (ADS)

Harrel, Shayne Matthew

Terahertz (THz) emission spectroscopy (TES) is newly developed experimental technique capable of measuring ultrafast dynamics in a variety of systems. Unlike pump-probe spectroscopies where the signals are obtained indirectly, the THz waveform emitted by the dynamical process serves as the signal field. Information about processes involving a time-dependent magnetization, polarization or current is obtained using TES. The detection scheme is polarization sensitive and allows the direction of the dynamical event to be recovered. The role of solvation on intramolecular charge transfer in DMANS (4-(dimethylamino)-4'-nitrostilbene) is studied using TES in three solvents: benzene, toluene, and 1,3-dichlorobenzene. These solvents have similar molecular structures but different polarities and dielectric constants. The charge transfer dynamics are found to depend on the solvent. A secondary feature in the THz emission appearing 4-6 Ps after the main pulse provides evidence that DMANS may undergo a twisted intramolecular charge transfer state (TICT) upon photoexcitation. The ultrafast magnetization dynamics of polycrystalline Ni and single Fe films ranging in thickness from 5 nm to 60 nm are reported using TES. For samples thicker than the visible optical skin depth, (˜10 nm for Ni and ˜27 nm for Fe), the emission is easily interpreted using Lenz's law. For films thinner than visible optical skin depth, the emission patterns are qualitatively different. These results suggest that there are two generation mechanisms at work: one that arises purely from bulk demagnetization in the thick sample limit and another that is the result of difference frequency generation enhanced by the magnetized surface. A comparative study of the magnetization dynamics of a 40 nm Ni and 40 Fe film shows that the magnetization recovers faster in Fe than in Ni. The dependence of optical rectification and shift currents in unbiased GaAs (111) is reported using TES. It is found that the dependence of the emission with respect to linear excitation polarization is well described by theory. The emission with respect to elliptical polarization also agrees well with theory when exciting below and far above the bandgap. However, the THz emission when exciting slightly above the bandgap is strongly influenced by spin-polarized electrons. The magnetic field generated by these spin-polarized electrons is responsible for altering their own trajectories via the self-induced Hall effect. The dependence of THz generation mechanisms in ZnTe (110) on excitation intensity is investigated using TES. Optical rectification is found to be the dominant generation mechanism only at the lowest excitation powers (<5 mW). A model of second harmonic induced shift currents generating THz radiation is unable to explain the emissions at higher excitation powers.

Optical resonance imaging: An optical analog to MRI with sub-diffraction-limited capabilities.

PubMed

Allodi, Marco A; Dahlberg, Peter D; Mazuski, Richard J; Davis, Hunter C; Otto, John P; Engel, Gregory S

2016-12-21

We propose here optical resonance imaging (ORI), a direct optical analog to magnetic resonance imaging (MRI). The proposed pulse sequence for ORI maps space to time and recovers an image from a heterodyne-detected third-order nonlinear photon echo measurement. As opposed to traditional photon echo measurements, the third pulse in the ORI pulse sequence has significant pulse-front tilt that acts as a temporal gradient. This gradient couples space to time by stimulating the emission of a photon echo signal from different lateral spatial locations of a sample at different times, providing a widefield ultrafast microscopy. We circumvent the diffraction limit of the optics by mapping the lateral spatial coordinate of the sample with the emission time of the signal, which can be measured to high precision using interferometric heterodyne detection. This technique is thus an optical analog of MRI, where magnetic-field gradients are used to localize the spin-echo emission to a point below the diffraction limit of the radio-frequency wave used. We calculate the expected ORI signal using 15 fs pulses and 87° of pulse-front tilt, collected using f /2 optics and find a two-point resolution 275 nm using 800 nm light that satisfies the Rayleigh criterion. We also derive a general equation for resolution in optical resonance imaging that indicates that there is a possibility of superresolution imaging using this technique. The photon echo sequence also enables spectroscopic determination of the input and output energy. The technique thus correlates the input energy with the final position and energy of the exciton.

Applications of telecommunication technology for optical instrumentation with an emphasis on space-time duality

NASA Astrophysics Data System (ADS)

van Howe, James William

Telecommunication technology has often been applied to areas of science and engineering seemingly unrelated to communication systems. Innovations such as electronic amplifiers, the transistor, digital coding, optical fiber, and the laser, which all had roots in communication technology, have been implemented in devices from bar-code scanners to fiber endoscopes for medical procedures. In the same way, the central theme of the work in the following chapters has been to borrow both the concepts and technology of telecommunications systems to develop novel optical instrumentation for non-telecom pursuits. This work particularly leverages fiber-integrated electro-optic phase modulators to apply custom phase profiles to ultrafast pulses for control and manipulation. Such devices are typically used in telecom transmitters to encode phase data onto optical pulses (differential phase-shift keying), or for chirped data transmission. We, however, use electro-optic phase modulators to construct four novel optical devices: (1) a programmable ultrafast optical delay line with record scanning speed for applications in optical metrology, interferometry, or broad-band phase arrays, (2) a multiwavelength pulse generator for real-time optical sampling of electronic waveforms, (3) a simple femtosecond pulse generator for uses in biomedical imaging or ultrafast spectroscopy, and (4) a nonlinear phase compensator to increase the energy of fiber-amplified ultrashort pulse systems. In addition, we describe a fifth instrument which makes use of a higher-order mode fiber, similar in design to dispersion compensating fibers used for telecom. Through soliton self-frequency shift in the higher-order mode fiber, we can broadly-tune the center frequency of ultrashort pulses in energy regimes useful for biomedical imaging or ultrafast spectroscopy. The advantages gained through using telecom components in each of these systems are the simplicity and robustness of all-fiber configurations, high-speed operation, and electronic control of signals. Finally, we devote much attention to the paradigm of space-time duality and temporal imaging which allows the electro-optic phase modulators used in our instrumentation to be framed as temporal analogs of diffractive optical elements such as lenses and prisms. We show how the concepts of "time-lenses" and "time-prisms" give an intuitive understanding of our work as well as insight for the general development of optical instrumentation.

Parametric spectro-temporal analyzer (PASTA) for ultrafast optical performance monitoring

NASA Astrophysics Data System (ADS)

Zhang, Chi; Wong, Kenneth K. Y.

2013-12-01

Ultrafast optical spectrum monitoring is one of the most challenging tasks in observing ultrafast phenomena, such as the spectroscopy, dynamic observation of the laser cavity, and spectral encoded imaging systems. However, conventional method such as optical spectrum analyzer (OSA) spatially disperses the spectrum, but the space-to-time mapping is realized by mechanical rotation of a grating, so are incapable of operating at high speed. Besides the spatial dispersion, temporal dispersion provided by dispersive fiber can also stretches the spectrum in time domain in an ultrafast manner, but is primarily confined in measuring short pulses. In view of these constraints, here we present a real-time spectrum analyzer called parametric spectro-temporal analyzer (PASTA), which is based on the time-lens focusing mechanism. It achieves a 100-MHz frame rate and can measure arbitrary waveforms. For the first time, we observe the dynamic spectrum of an ultrafast swept-source: Fourier domain mode-locked (FDML) laser, and the spectrum evolution of a laser cavity during its stabilizing process. In addition to the basic single-lens structure, the multi-lens configurations (e.g. telescope or wide-angle scope) will provide a versatile operating condition, which can zoom in to achieve 0.05-nm resolution and zoom out to achieve 10-nm observation range, namely 17 times zoom in/out ratio. In view of the goal of achieving spectrum analysis with fine accuracy, PASTA provides a promising path to study the real-time spectrum of some dynamic phenomena and non-repetitive events, with orders of magnitude enhancement in the frame rate over conventional OSAs.

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy

PubMed Central

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H.

2014-01-01

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material’s electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier–carrier scatterings which are mirrored in the energy of material’s secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces. PMID:24469803

Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy.

PubMed

Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H

2014-02-11

Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material's electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier-carrier scatterings which are mirrored in the energy of material's secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces.

Spatially confined low-power optically pumped ultrafast synchrotron x-ray nanodiffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Joonkyu; Zhang, Qingteng; Chen, Pice

2015-08-27

The combination of ultrafast optical excitation and time-resolved synchrotron x-ray nanodiffraction provides unique insight into the photoinduced dynamics of materials, with the spatial resolution required to probe individual nanostructures or small volumes within heterogeneous materials. Optically excited x-ray nanobeam experiments are challenging because the high total optical power required for experimentally relevant optical fluences leads to mechanical instability due to heating. For a given fluence, tightly focusing the optical excitation reduces the average optical power by more than three orders of magnitude and thus ensures sufficient thermal stability for x-ray nanobeam studies. Delivering optical pulses via a scannable fiber-coupled opticalmore » objective provides a well-defined excitation geometry during rotation and translation of the sample and allows the selective excitation of isolated areas within the sample. Finally, experimental studies of the photoinduced lattice dynamics of a 35 nm BiFeO 3 thin film on a SrTiO 3 substrate demonstrate the potential to excite and probe nanoscale volumes.« less

Wavelength-encoded tomography based on optical temporal Fourier transform

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Chi; Wong, Kenneth K. Y., E-mail: kywong@eee.hku.hk

We propose and demonstrate a technique called wavelength-encoded tomography (WET) for non-invasive optical cross-sectional imaging, particularly beneficial in biological system. The WET utilizes time-lens to perform the optical Fourier transform, and the time-to-wavelength conversion generates a wavelength-encoded image of optical scattering from internal microstructures, analogous to the interferometery-based imaging such as optical coherence tomography. Optical Fourier transform, in principle, comes with twice as good axial resolution over the electrical Fourier transform, and will greatly simplify the digital signal processing after the data acquisition. As a proof-of-principle demonstration, a 150 -μm (ideally 36 μm) resolution is achieved based on a 7.5-nm bandwidth swept-pump,more » using a conventional optical spectrum analyzer. This approach can potentially achieve up to 100-MHz or even higher frame rate with some proven ultrafast spectrum analyzer. We believe that this technique is innovative towards the next-generation ultrafast optical tomographic imaging application.« less

Full Stark control of polariton states on a spin-orbit hypersphere

NASA Astrophysics Data System (ADS)

Li, Feng; Cancellieri, E.; Buonaiuto, G.; Skolnick, M. S.; Krizhanovskii, D. N.; Whittaker, D. M.

2016-11-01

The orbital angular momentum and the polarization of light are physical quantities widely investigated for classical and quantum information processing. In this work we propose to take advantage of strong light-matter coupling, circular-symmetric confinement, and transverse-electric transverse-magnetic splitting to exploit states where these two degrees of freedom are combined. To this end we develop a model based on a spin-orbit Poincaré hypersphere. Then we consider the example of semiconductor polariton systems and demonstrate full ultrafast Stark control of spin-orbit states. Moreover, by controlling states on three different spin-orbit spheres and switching from one sphere to another we demonstrate the control of different logic bits within one single physical system.

650-nJ pulses from a cavity-dumped Yb:fiber-pumped ultrafast optical parametric oscillator

NASA Astrophysics Data System (ADS)

Lamour, Tobias P.; Reid, Derryck T.

2011-08-01

Sub-250-fs pulses with energies of up to 650 nJ and peak powers up to 2.07 MW were generated from a cavity-dumped optical parametric oscillator, synchronously-pumped at 15.3 MHz with sub-400-fs pulses from an Yb:fiber laser. The average beam quality factor of the dumped output was M2 ~1.2 and the total relative-intensity noise was 8 mdBc, making the system a promising candidate for ultrafast laser inscription of infrared materials.

Ultrafast Optical Modulation of Second- and Third-Harmonic Generation from Cut-Disk-Based Metasurfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sartorello, Giovanni; Olivier, Nicolas; Zhang, Jingjing

2016-08-17

We design and fabricate a metasurface composed of gold cut-disk resonators that exhibits a strong coherent nonlinear response. We experimentally demonstrate all-optical modulation of both second- and third-harmonic signals on a subpicosecond time scale. Pump probe experiments and numerical models show that the observed effects are due to the ultrafast response of the electronic excitations in the metal under external illumination. These effects pave the way for the development of novel active nonlinear metasurfaces with controllable and switchable coherent nonlinear response.

OSA Proceedings on Ultrafast Electronics and Optoelectronics Held in San Francisco, California on January 25 -27, 1993. Volume 14,

DTIC Science & Technology

1993-01-27

Venkatesan, Zhi- Yuan Shen, Philip Pang, Dennis J. Kountz, and William L Holstein Response of a Nb/A1203/Nb Tunnel Junction to Picosecond Electrical Pulses...Mwhra (edo) 0 1993 Optical Sockty ofAnierica 152 Ultrafast Electronics and Optoelectronics core cladding COW MAD 75. 4UHN 1058nm 50Ps A A optical...Maryland. College Park; Maryland 20742 7hi-Yuan Shen, Philip Pang, Dennis J. Kountz, and William L. Holstein Central Research and Development, Du Pont, PO

Ultrafast frequency-agile terahertz devices using methylammonium lead halide perovskites

PubMed Central

Chanana, Ashish; Liu, Xiaojie; Vardeny, Zeev Valy

2018-01-01

The ability to control the response of metamaterial structures can facilitate the development of new terahertz devices, with applications in spectroscopy and communications. We demonstrate ultrafast frequency-agile terahertz metamaterial devices that enable such a capability, in which multiple perovskites can be patterned in each unit cell with micrometer-scale precision. To accomplish this, we developed a fabrication technique that shields already deposited perovskites from organic solvents, allowing for multiple perovskites to be patterned in close proximity. By doing so, we demonstrate tuning of the terahertz resonant response that is based not only on the optical pump fluence but also on the optical wavelength. Because polycrystalline perovskites have subnanosecond photocarrier recombination lifetimes, switching between resonances can occur on an ultrafast time scale. The use of multiple perovskites allows for new functionalities that are not possible using a single semiconducting material. For example, by patterning one perovskite in the gaps of split-ring resonators and bringing a uniform thin film of a second perovskite in close proximity, we demonstrate tuning of the resonant response using one optical wavelength and suppression of the resonance using a different optical wavelength. This general approach offers new capabilities for creating tunable terahertz devices. PMID:29736416

Ultrafast frequency-agile terahertz devices using methylammonium lead halide perovskites.

PubMed

Chanana, Ashish; Liu, Xiaojie; Zhang, Chuang; Vardeny, Zeev Valy; Nahata, Ajay

2018-05-01

The ability to control the response of metamaterial structures can facilitate the development of new terahertz devices, with applications in spectroscopy and communications. We demonstrate ultrafast frequency-agile terahertz metamaterial devices that enable such a capability, in which multiple perovskites can be patterned in each unit cell with micrometer-scale precision. To accomplish this, we developed a fabrication technique that shields already deposited perovskites from organic solvents, allowing for multiple perovskites to be patterned in close proximity. By doing so, we demonstrate tuning of the terahertz resonant response that is based not only on the optical pump fluence but also on the optical wavelength. Because polycrystalline perovskites have subnanosecond photocarrier recombination lifetimes, switching between resonances can occur on an ultrafast time scale. The use of multiple perovskites allows for new functionalities that are not possible using a single semiconducting material. For example, by patterning one perovskite in the gaps of split-ring resonators and bringing a uniform thin film of a second perovskite in close proximity, we demonstrate tuning of the resonant response using one optical wavelength and suppression of the resonance using a different optical wavelength. This general approach offers new capabilities for creating tunable terahertz devices.

Ultrafast light matter interaction in CdSe/ZnS core-shell quantum dots

NASA Astrophysics Data System (ADS)

Yadav, Rajesh Kumar; Sharma, Rituraj; Mondal, Anirban; Adarsh, K. V.

2018-04-01

Core-shell quantum dot are imperative for carrier (electron and holes) confinement in core/shell, which provides a stage to explore the linear and nonlinear optical phenomena at the nanoscalelimit. Here we present a comprehensive study of ultrafast excitation dynamics and nonlinear optical absorption of CdSe/ZnS core shell quantum dot with the help of ultrafast spectroscopy. Pump-probe and time-resolved measurements revealed the drop of trapping at CdSe surface due to the presence of the ZnS shell, which makes more efficient photoluminescence. We have carried out femtosecond transient absorption studies of the CdSe/ZnS core-shell quantum dot by irradiation with 400 nm laser light, monitoring the transients in the visible region. The optical nonlinearity of the core-shell quantum dot studied by using the Z-scan technique with 120 fs pulses at the wavelengths of 800 nm. The value of two photon absorption coefficients (β) of core-shell QDs extracted as80cm/GW, and it shows excellent benchmark for the optical limiting onset of 2.5GW/cm2 with the low limiting differential transmittance of 0.10, that is an order of magnitude better than graphene based materials.

Terahertz spin current pulses controlled by magnetic heterostructures

NASA Astrophysics Data System (ADS)

Kampfrath, T.; Battiato, M.; Maldonado, P.; Eilers, G.; Nötzold, J.; Mährlein, S.; Zbarsky, V.; Freimuth, F.; Mokrousov, Y.; Blügel, S.; Wolf, M.; Radu, I.; Oppeneer, P. M.; Münzenberg, M.

2013-04-01

In spin-based electronics, information is encoded by the spin state of electron bunches. Processing this information requires the controlled transport of spin angular momentum through a solid, preferably at frequencies reaching the so far unexplored terahertz regime. Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is used to drive spins from a ferromagnetic iron thin film into a non-magnetic cap layer that has either low (ruthenium) or high (gold) electron mobility. The resulting transient spin current is detected by means of an ultrafast, contactless amperemeter based on the inverse spin Hall effect, which converts the spin flow into a terahertz electromagnetic pulse. We find that the ruthenium cap layer yields a considerably longer spin current pulse because electrons are injected into ruthenium d states, which have a much lower mobility than gold sp states. Thus, spin current pulses and the resulting terahertz transients can be shaped by tailoring magnetic heterostructures, which opens the door to engineering high-speed spintronic devices and, potentially, broadband terahertz emitters.

New opportunities at the frontiers of spintronics

DOE PAGES

Hoffmann, Axel; Bader, Sam D.

2015-10-05

The field of spintronics, or magnetic electronics, is maturing and giving rise to new subfields. These new directions involve the study of collective spin excitations and couplings of the spin system to additional degrees of freedom of a material, as well as metastable phenomena due to perturbations that drive the system far from equilibrium. The interactions lead to possibilities for future applications within the realm of energy-efficient information technologies. Examples discussed herein include research opportunities associated with (i) various spin-orbit couplings, such as spin Hall effects, (ii) couplings to the thermal bath of a system, such as in spin Seebeckmore » effects, (iii) spin-spin couplings, such as via induced and interacting magnon excitations, and (iv) spin-photon couplings, such as in ultra-fast magnetization switching due to coherent photon pulses. These four basic frontier areas of research are giving rise to new applied disciplines known as spin-orbitronics, spin-caloritronics, magnonics, and spin-photonics, respectively. These topics are highlighted in order to stimulate interest in the new directions that spintronics research is taking, and to identify open issues to pursue.« less

Excited state dynamics & optical control of molecular motors

NASA Astrophysics Data System (ADS)

Wiley, Ted; Sension, Roseanne

2014-03-01

Chiral overcrowded alkenes are likely candidates for light driven rotary molecular motors. At their core, these molecular motors are based on the chromophore stilbene, undergoing ultrafast cis/trans photoisomerization about their central double bond. Unlike stilbene, the photochemistry of molecular motors proceeds in one direction only. This unidirectional rotation is a result of helicity in the molecule induced by steric hindrance. However, the steric hindrance which ensures unidirectional excited state rotation, has the unfortunate consequence of producing large ground state barriers which dramatically decrease the overall rate of rotation. These molecular scale ultrafast motors have only recently been studied by ultrafast spectroscopy. Our lab has studied the photochemistry and photophysics of a ``first generation'' molecular motor with UV-visible transient absorption spectroscopy. We hope to use optical pulse shaping to enhance the efficiency and turnover rate of these molecular motors.

WS2 mode-locked ultrafast fiber laser

PubMed Central

Mao, Dong; Wang, Yadong; Ma, Chaojie; Han, Lei; Jiang, Biqiang; Gan, Xuetao; Hua, Shijia; Zhang, Wending; Mei, Ting; Zhao, Jianlin

2015-01-01

Graphene-like two dimensional materials, such as WS2 and MoS2, are highly anisotropic layered compounds that have attracted growing interest from basic research to practical applications. Similar with MoS2, few-layer WS2 has remarkable physical properties. Here, we demonstrate for the first time that WS2 nanosheets exhibit ultrafast nonlinear saturable absorption property and high optical damage threshold. Soliton mode-locking operations are achieved separately in an erbium-doped fiber laser using two types of WS2-based saturable absorbers, one of which is fabricated by depositing WS2 nanosheets on a D-shaped fiber, while the other is synthesized by mixing WS2 solution with polyvinyl alcohol, and then evaporating them on a substrate. At the maximum pump power of 600 mW, two saturable absorbers can work stably at mode-locking state without damage, indicating that few-layer WS2 is a promising high-power flexible saturable absorber for ultrafast optics. Numerous applications may benefit from the ultrafast nonlinear features of WS2 nanosheets, such as high-power pulsed laser, materials processing, and frequency comb spectroscopy. PMID:25608729

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy

PubMed Central

Feist, Armin; Rubiano da Silva, Nara; Liang, Wenxi; Ropers, Claus; Schäfer, Sascha

2018-01-01

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction with a nanoscale probe beam for the quantitative retrieval of the time-dependent local deformation gradient tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels. PMID:29464187

Filter-Based Dispersion-Managed Versatile Ultrafast Fibre Laser

PubMed Central

Peng, Junsong; Boscolo, Sonia

2016-01-01

We present the operation of an ultrafast passively mode-locked fibre laser, in which flexible control of the pulse formation mechanism is readily realised by an in-cavity programmable filter the dispersion and bandwidth of which can be software configured. We show that conventional soliton, dispersion-managed (DM) soliton (stretched-pulse) and dissipative soliton mode-locking regimes can be reliably targeted by changing the filter’s dispersion and bandwidth only, while no changes are made to the physical layout of the laser cavity. Numerical simulations are presented which confirm the different nonlinear pulse evolutions inside the laser cavity. The proposed technique holds great potential for achieving a high degree of control over the dynamics and output of ultrafast fibre lasers, in contrast to the traditional method to control the pulse formation mechanism in a DM fibre laser, which involves manual optimisation of the relative length of fibres with opposite-sign dispersion in the cavity. Our versatile ultrafast fibre laser will be attractive for applications requiring different pulse profiles such as in optical signal processing and optical communications. PMID:27183882

Nanoscale diffractive probing of strain dynamics in ultrafast transmission electron microscopy.

PubMed

Feist, Armin; Rubiano da Silva, Nara; Liang, Wenxi; Ropers, Claus; Schäfer, Sascha

2018-01-01

The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction with a nanoscale probe beam for the quantitative retrieval of the time-dependent local deformation gradient tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformations close to the edge of a single-crystalline graphite membrane. Tracking the structural distortion with a 28-nm/700-fs spatio-temporal resolution, we observe an acoustic membrane breathing mode with spatially modulated amplitude, governed by the optical near field structure at the membrane edge. Furthermore, an in-plane polarized acoustic shock wave is launched at the membrane edge, which triggers secondary acoustic shear waves with a pronounced spatio-temporal dependency. The experimental findings are compared to numerical acoustic wave simulations in the continuous medium limit, highlighting the importance of microscopic dissipation mechanisms and ballistic transport channels.

Low-threshold ultrafast all-optical switch implemented with metallic nanoshells in the photonic crystal ring resonator

NASA Astrophysics Data System (ADS)

Ghadrdan, Majid; Mansouri-Birjandi, Mohammad Ali

2017-11-01

An all-optical switch based on nonlinear photonic crystal ring resonator embedded with silica dielectric surrounded by silver nanoshell (NS) inside the ring resonator has been introduced and analyzed in this article. We considered silica with radius of 10 nm and silver with radius of 16 nm as core and shell, respectively. By placing NSs inside the photonic crystal ring resonator, we succeeded in reducing the threshold power to 12.8 mW/μm2 and the switching time to about 0.4 ps. The results of this research suggest a new technique for reducing switching light intensity. With small size, ultra-fast switching time, and low-threshold power, the structure has the potential to be applied in optical integration circuits and nanoscale optical chips.

Nonlinear ultrafast optical response in organic molecular crystals

NASA Astrophysics Data System (ADS)

Rahman, Talat S.; Turkowski, Volodymyr; Leuenberger, Michael N.

2012-02-01

We analyze possible nonlinear excitonic effects in the organic molecule crystals by using a combined time-dependent DFT and many-body approach. In particular, we analyze possible effects of the time-dependent (retarded)interaction between different types of excitations, Frenkel excitons, charge transfer excitons and excimers, on the electric and the optical response of the system. We pay special attention to the case of constant electric field and ultrafast pulses, including that of four-wave mixing experiments. As a specific application we examine the optical excitations of pentacene nanocrystals and compare the results with available experimental data.[1] Our results demostrate that the nonlinear effects can play an important role in the optical response of these systems. [1] A. Kabakchiev, ``Scanning Tunneling Luminescence of Pentacene Nanocrystals'', PhD Thesis (EPFL, Lausanne, 2010).

Solution-assisted ultrafast transfer of graphene-based thin films for solar cells and humidity sensors.

PubMed

Sun, Jiawei; Xie, Xiao; Bi, Hengchang; Jia, Haiyang; Zhu, Chongyang; Wan, Neng; Huang, Jianqiu; Nie, Meng; Li, Dan; Sun, Litao

2017-03-01

Vacuum filtration enables the fabrication of large-area graphene-based membranes (GBMs), possessing a smoother surface than that by spray, spin coating or drop casting. However, due to the strong interaction with substrates, the separation of thin GBMs from the filter is problematic. Conventional stamping separation/transfer of graphene oxide (GO) thin films requires another substrate and pressing for >10 h, which may damage the delicate structure of the transfer substrates. Other methods require GO to be reduced on filters before separation, thus limiting the reduction methods. Inspired by a coagulation bath that enables rapid formation of ultrastrong GO fibers, we present an ultrafast (<1 min) and solution-assisted strategy to fabricate smooth and freestanding GO films. The diverse interfacial energy of hydrogen bonds also demonstrates another reason for the successful separation. The film thickness ranges from 45 nm to several micrometers. When used as a composite of counter electrodes in dye sensitized solar cells, it showed higher (8.58%) power conversion efficiency than its spin-(7.71%) and spray-coated (8.07%) counterparts. It also showed promising performance in capacitive humidity sensors. The capacitance varied by three orders of magnitude in the range of the relative humidity of 15%-95%. Therefore the strategy realizes an ultrafast and high-quality film production which is suitable for various applications.

Solution-assisted ultrafast transfer of graphene-based thin films for solar cells and humidity sensors

NASA Astrophysics Data System (ADS)

Sun, Jiawei; Xie, Xiao; Bi, Hengchang; Jia, Haiyang; Zhu, Chongyang; Wan, Neng; Huang, Jianqiu; Nie, Meng; Li, Dan; Sun, Litao

2017-03-01

Vacuum filtration enables the fabrication of large-area graphene-based membranes (GBMs), possessing a smoother surface than that by spray, spin coating or drop casting. However, due to the strong interaction with substrates, the separation of thin GBMs from the filter is problematic. Conventional stamping separation/transfer of graphene oxide (GO) thin films requires another substrate and pressing for >10 h, which may damage the delicate structure of the transfer substrates. Other methods require GO to be reduced on filters before separation, thus limiting the reduction methods. Inspired by a coagulation bath that enables rapid formation of ultrastrong GO fibers, we present an ultrafast (<1 min) and solution-assisted strategy to fabricate smooth and freestanding GO films. The diverse interfacial energy of hydrogen bonds also demonstrates another reason for the successful separation. The film thickness ranges from 45 nm to several micrometers. When used as a composite of counter electrodes in dye sensitized solar cells, it showed higher (8.58%) power conversion efficiency than its spin-(7.71%) and spray-coated (8.07%) counterparts. It also showed promising performance in capacitive humidity sensors. The capacitance varied by three orders of magnitude in the range of the relative humidity of 15%-95%. Therefore the strategy realizes an ultrafast and high-quality film production which is suitable for various applications.

Real-time visualization of soliton molecules with evolving behavior in an ultrafast fiber laser

NASA Astrophysics Data System (ADS)

Liu, Meng; Li, Heng; Luo, Ai-Ping; Cui, Hu; Xu, Wen-Cheng; Luo, Zhi-Chao

2018-03-01

Ultrafast fiber lasers have been demonstrated to be great platforms for the investigation of soliton dynamics. The soliton molecules, as one of the most fascinating nonlinear phenomena, have been a hot topic in the field of nonlinear optics in recent years. Herein, we experimentally observed the real-time evolving behavior of soliton molecule in an ultrafast fiber laser by using the dispersive Fourier transformation technology. Several types of evolving soliton molecules were obtained in our experiments, such as soliton molecules with monotonically or chaotically evolving phase, flipping and hopping phase. These results would be helpful to the communities interested in soliton nonlinear dynamics as well as ultrafast laser technologies.

Spin-orbit torque induced magnetic vortex polarity reversal utilizing spin-Hall effect

NASA Astrophysics Data System (ADS)

Li, Cheng; Cai, Li; Liu, Baojun; Yang, Xiaokuo; Cui, Huanqing; Wang, Sen; Wei, Bo

2018-05-01

We propose an effective magnetic vortex polarity reversal scheme that makes use of spin-orbit torque introduced by spin-Hall effect in heavy-metal/ferromagnet multilayers structure, which can result in subnanosecond polarity reversal without endangering the structural stability. Micromagnetic simulations are performed to investigate the spin-Hall effect driven dynamics evolution of magnetic vortex. The mechanism of magnetic vortex polarity reversal is uncovered by a quantitative analysis of exchange energy density, magnetostatic energy density, and their total energy density. The simulation results indicate that the magnetic vortex polarity is reversed through the nucleation-annihilation process of topological vortex-antivortex pair. This scheme is an attractive option for ultra-fast magnetic vortex polarity reversal, which can be used as the guidelines for the choice of polarity reversal scheme in vortex-based random access memory.

Ultrafast Microfluidic Cellular Imaging by Optical Time-Stretch.

PubMed

Lau, Andy K S; Wong, Terence T W; Shum, Ho Cheung; Wong, Kenneth K Y; Tsia, Kevin K

2016-01-01

There is an unmet need in biomedicine for measuring a multitude of parameters of individual cells (i.e., high content) in a large population efficiently (i.e., high throughput). This is particularly driven by the emerging interest in bringing Big-Data analysis into this arena, encompassing pathology, drug discovery, rare cancer cell detection, emulsion microdroplet assays, to name a few. This momentum is particularly evident in recent advancements in flow cytometry. They include scaling of the number of measurable colors from the labeled cells and incorporation of imaging capability to access the morphological information of the cells. However, an unspoken predicament appears in the current technologies: higher content comes at the expense of lower throughput, and vice versa. For example, accessing additional spatial information of individual cells, imaging flow cytometers only achieve an imaging throughput ~1000 cells/s, orders of magnitude slower than the non-imaging flow cytometers. In this chapter, we introduce an entirely new imaging platform, namely optical time-stretch microscopy, for ultrahigh speed and high contrast label-free single-cell (in a ultrafast microfluidic flow up to 10 m/s) imaging and analysis with an ultra-fast imaging line-scan rate as high as tens of MHz. Based on this technique, not only morphological information of the individual cells can be obtained in an ultrafast manner, quantitative evaluation of cellular information (e.g., cell volume, mass, refractive index, stiffness, membrane tension) at nanometer scale based on the optical phase is also possible. The technology can also be integrated with conventional fluorescence measurements widely adopted in the non-imaging flow cytometers. Therefore, these two combinatorial and complementary measurement capabilities in long run is an attractive platform for addressing the pressing need for expanding the "parameter space" in high-throughput single-cell analysis. This chapter provides the general guidelines of constructing the optical system for time stretch imaging, fabrication and design of the microfluidic chip for ultrafast fluidic flow, as well as the image acquisition and processing.

Ultrafast ultrasound localization microscopy for deep super-resolution vascular imaging

NASA Astrophysics Data System (ADS)

Errico, Claudia; Pierre, Juliette; Pezet, Sophie; Desailly, Yann; Lenkei, Zsolt; Couture, Olivier; Tanter, Mickael

2015-11-01

Non-invasive imaging deep into organs at microscopic scales remains an open quest in biomedical imaging. Although optical microscopy is still limited to surface imaging owing to optical wave diffusion and fast decorrelation in tissue, revolutionary approaches such as fluorescence photo-activated localization microscopy led to a striking increase in resolution by more than an order of magnitude in the last decade. In contrast with optics, ultrasonic waves propagate deep into organs without losing their coherence and are much less affected by in vivo decorrelation processes. However, their resolution is impeded by the fundamental limits of diffraction, which impose a long-standing trade-off between resolution and penetration. This limits clinical and preclinical ultrasound imaging to a sub-millimetre scale. Here we demonstrate in vivo that ultrasound imaging at ultrafast frame rates (more than 500 frames per second) provides an analogue to optical localization microscopy by capturing the transient signal decorrelation of contrast agents—inert gas microbubbles. Ultrafast ultrasound localization microscopy allowed both non-invasive sub-wavelength structural imaging and haemodynamic quantification of rodent cerebral microvessels (less than ten micrometres in diameter) more than ten millimetres below the tissue surface, leading to transcranial whole-brain imaging within short acquisition times (tens of seconds). After intravenous injection, single echoes from individual microbubbles were detected through ultrafast imaging. Their localization, not limited by diffraction, was accumulated over 75,000 images, yielding 1,000,000 events per coronal plane and statistically independent pixels of ten micrometres in size. Precise temporal tracking of microbubble positions allowed us to extract accurately in-plane velocities of the blood flow with a large dynamic range (from one millimetre per second to several centimetres per second). These results pave the way for deep non-invasive microscopy in animals and humans using ultrasound. We anticipate that ultrafast ultrasound localization microscopy may become an invaluable tool for the fundamental understanding and diagnostics of various disease processes that modify the microvascular blood flow, such as cancer, stroke and arteriosclerosis.

Ultrafast ultrasound localization microscopy for deep super-resolution vascular imaging.

PubMed

Errico, Claudia; Pierre, Juliette; Pezet, Sophie; Desailly, Yann; Lenkei, Zsolt; Couture, Olivier; Tanter, Mickael

2015-11-26

Non-invasive imaging deep into organs at microscopic scales remains an open quest in biomedical imaging. Although optical microscopy is still limited to surface imaging owing to optical wave diffusion and fast decorrelation in tissue, revolutionary approaches such as fluorescence photo-activated localization microscopy led to a striking increase in resolution by more than an order of magnitude in the last decade. In contrast with optics, ultrasonic waves propagate deep into organs without losing their coherence and are much less affected by in vivo decorrelation processes. However, their resolution is impeded by the fundamental limits of diffraction, which impose a long-standing trade-off between resolution and penetration. This limits clinical and preclinical ultrasound imaging to a sub-millimetre scale. Here we demonstrate in vivo that ultrasound imaging at ultrafast frame rates (more than 500 frames per second) provides an analogue to optical localization microscopy by capturing the transient signal decorrelation of contrast agents--inert gas microbubbles. Ultrafast ultrasound localization microscopy allowed both non-invasive sub-wavelength structural imaging and haemodynamic quantification of rodent cerebral microvessels (less than ten micrometres in diameter) more than ten millimetres below the tissue surface, leading to transcranial whole-brain imaging within short acquisition times (tens of seconds). After intravenous injection, single echoes from individual microbubbles were detected through ultrafast imaging. Their localization, not limited by diffraction, was accumulated over 75,000 images, yielding 1,000,000 events per coronal plane and statistically independent pixels of ten micrometres in size. Precise temporal tracking of microbubble positions allowed us to extract accurately in-plane velocities of the blood flow with a large dynamic range (from one millimetre per second to several centimetres per second). These results pave the way for deep non-invasive microscopy in animals and humans using ultrasound. We anticipate that ultrafast ultrasound localization microscopy may become an invaluable tool for the fundamental understanding and diagnostics of various disease processes that modify the microvascular blood flow, such as cancer, stroke and arteriosclerosis.

Low-power, ultrafast, and dynamic all-optical tunable plasmon induced transparency in two stub resonators side-coupled with a plasmonic waveguide system

NASA Astrophysics Data System (ADS)

Wang, Boyun; Zeng, Qingdong; Xiao, Shuyuan; Xu, Chen; Xiong, Liangbin; Lv, Hao; Du, Jun; Yu, Huaqing

2017-11-01

We theoretically and numerically investigate a low-power, ultrafast, and dynamic all-optical tunable plasmon induced transparency (PIT) in two stub resonators side-coupled with a metal-dielectric-metal (MDM) plasmonic waveguide system. The optical Kerr effect is enhanced by the local electromagnetic field of surface plasmon polaritons (SPPs) and the plasmonic waveguide based on graphene-Ag composite material structures with large effective Kerr nonlinear coefficient. An ultrafast response time of the order of 1 ps is reached because of ultrafast carrier relaxation dynamics of graphene. With dynamically tuning the propagation phase of the plasmonic waveguide, π-phase shift of the transmission spectrum in the PIT system is achieved under excitation of a pump light with an intensity as low as 5.8 MW cm-2. The group delay is controlled between 0.14 and 0.67 ps. Moreover, the tunable bandwidth of about 42 nm is obtained. For the indirect coupling between two stub cavities or the phase coupling scheme, the phase shift multiplication effect of the PIT effect is found. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. This work not only paves the way towards the realization of on-chip integrated nanophotonic devices but also opens the possibility of the construction of ultrahigh-speed information processing chips based on plasmonic circuits.

Electro-optic deflectors deliver advantages over acousto-optical deflectors in a high resolution, ultra-fast force-clamp optical trap.

PubMed

Woody, Michael S; Capitanio, Marco; Ostap, E Michael; Goldman, Yale E

2018-04-30

We characterized experimental artifacts arising from the non-linear response of acousto-optical deflectors (AODs) in an ultra-fast force-clamp optical trap and have shown that using electro-optical deflectors (EODs) instead eliminates these artifacts. We give an example of the effects of these artifacts in our ultra-fast force clamp studies of the interaction of myosin with actin filaments. The experimental setup, based on the concept of Capitanio et al. [Nat. Methods 9, 1013-1019 (2012)] utilizes a bead-actin-bead dumbbell held in two force-clamped optical traps which apply a load to the dumbbell to move it at a constant velocity. When myosin binds to actin, the filament motion stops quickly as the total force from the optical traps is transferred to the actomyosin attachment. We found that in our setup, AODs were unsuitable for beam steering due to non-linear variations in beam intensity and deflection angle as a function of driving frequency, likely caused by low-amplitude standing acoustic waves in the deflectors. These aberrations caused instability in the force feedback loops leading to artifactual jumps in the trap position. We demonstrate that beam steering with EODs improves the performance of our instrument. Combining the superior beam-steering capability of the EODs, force acquisition via back-focal-plane interferometry, and dual high-speed FPGA-based feedback loops, we apply precise and constant loads to study the dynamics of interactions between actin and myosin. The same concept applies to studies of other biomolecular interactions.

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources.

PubMed

Pincelli, T; Petrov, V N; Brajnik, G; Ciprian, R; Lollobrigida, V; Torelli, P; Krizmancic, D; Salvador, F; De Luisa, A; Sergo, R; Gubertini, A; Cautero, G; Carrato, S; Rossi, G; Panaccione, G

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

NASA Astrophysics Data System (ADS)

Pincelli, T.; Petrov, V. N.; Brajnik, G.; Ciprian, R.; Lollobrigida, V.; Torelli, P.; Krizmancic, D.; Salvador, F.; De Luisa, A.; Sergo, R.; Gubertini, A.; Cautero, G.; Carrato, S.; Rossi, G.; Panaccione, G.

2016-03-01

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric and magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).

Design and optimization of a modular setup for measurements of three-dimensional spin polarization with ultrafast pulsed sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pincelli, T., E-mail: pincelli@iom.cnr.it; Rossi, G.; Laboratorio TASC, IOM-CNR, S.S. 14 km 163.5, Basovizza, 34149 Trieste

2016-03-15

ULTRASPIN is an apparatus devoted to the measurement of the spin polarization (SP) of electrons ejected from solid surfaces in a UHV environment. It is designed to exploit ultrafast light sources (free electron laser or laser high harmonic generation) and to perform (photo)electron spin analysis by an arrangement of Mott scattering polarimeters that measure the full SP vector. The system consists of two interconnected UHV vessels: one for surface science sample cleaning treatments, e-beam deposition of ultrathin films, and low energy electron diffraction/AES characterization. The sample environment in the polarimeter allows for cryogenic cooling and in-operando application of electric andmore » magnetic fields. The photoelectrons are collected by an electrostatic accelerator and transport lens that form a periaxial beam that is subsequently directed by a Y-shaped electrostatic deflector to either one of the two orthogonal Mott polarimeters. The apparatus has been designed to operate in the extreme conditions of ultraintense single-X-ray pulses as originated by free electron lasers (up to 1 kHz), but it allows also for the single electron counting mode suitable when using statistical sources such as synchrotron radiation, cw-laser, or e-gun beams (up to 150 kcps).« less

An ultrafast electron microscope gun driven by two-photon photoemission from a nanotip cathode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bormann, Reiner; Strauch, Stefanie; Schäfer, Sascha, E-mail: schaefer@ph4.physik.uni-goettingen.de

We experimentally and numerically investigate the performance of an advanced ultrafast electron source, based on two-photon photoemission from a tungsten needle cathode incorporated in an electron microscope gun geometry. Emission properties are characterized as a function of the electrostatic gun settings, and operating conditions leading to laser-triggered electron beams of very low emittance (below 20 nm mrad) are identified. The results highlight the excellent suitability of optically driven nano-cathodes for the further development of ultrafast transmission electron microscopy.

Cross-phase modulation bandwidth in ultrafast fiber wavelength converters

NASA Astrophysics Data System (ADS)

Luís, Ruben S.; Monteiro, Paulo; Teixeira, António

2006-12-01

We propose a novel analytical model for the characterization of fiber cross-phase modulation (XPM) in ultrafast all-optical fiber wavelength converters, operating at modulation frequencies higher than 1THz. The model is used to compare the XPM frequency limitations of a conventional and a highly nonlinear dispersion shifted fiber (HN-DSF) and a bismuth oxide-based fiber, introducing the XPM bandwidth as a design parameter. It is shown that the HN-DSF presents the highest XPM bandwidth, above 1THz, making it the most appropriate for ultrafast wavelength conversion.

Acousto-Optic Tunable Filter for Time-Domain Processing of Ultra-Short Optical Pulses,

DTIC Science & Technology

The application of acousto - optic tunable filters for shaping of ultra-fast pulses in the time domain is analyzed and demonstrated. With the rapid...advance of acousto - optic tunable filter (AOTF) technology, the opportunity for sophisticated signal processing capabilities arises. AOTFs offer unique

Linear and ultrafast nonlinear plasmonics of single nano-objects

NASA Astrophysics Data System (ADS)

Crut, Aurélien; Maioli, Paolo; Vallée, Fabrice; Del Fatti, Natalia

2017-03-01

Single-particle optical investigations have greatly improved our understanding of the fundamental properties of nano-objects, avoiding the spurious inhomogeneous effects that affect ensemble experiments. Correlation with high-resolution imaging techniques providing morphological information (e.g. electron microscopy) allows a quantitative interpretation of the optical measurements by means of analytical models and numerical simulations. In this topical review, we first briefly recall the principles underlying some of the most commonly used single-particle optical techniques: near-field, dark-field, spatial modulation and photothermal microscopies/spectroscopies. We then focus on the quantitative investigation of the surface plasmon resonance (SPR) of metallic nano-objects using linear and ultrafast optical techniques. While measured SPR positions and spectral areas are found in good agreement with predictions based on Maxwell’s equations, SPR widths are strongly influenced by quantum confinement (or, from a classical standpoint, surface-induced electron scattering) and, for small nano-objects, cannot be reproduced using the dielectric functions of bulk materials. Linear measurements on single nano-objects (silver nanospheres and gold nanorods) allow a quantification of the size and geometry dependences of these effects in confined metals. Addressing the ultrafast response of an individual nano-object is also a powerful tool to elucidate the physical mechanisms at the origin of their optical nonlinearities, and their electronic, vibrational and thermal relaxation processes. Experimental investigations of the dynamical response of gold nanorods are shown to be quantitatively modeled in terms of modifications of the metal dielectric function enhanced by plasmonic effects. Ultrafast spectroscopy can also be exploited to unveil hidden physical properties of more complex nanosystems. In this context, two-color femtosecond pump-probe experiments performed on individual bimetallic heterodimers are discussed in the last part of the review, demonstrating the existence of Fano interferences in the optical absorption of a gold nanoparticle under the influence of a nearby silver one.

Ultrafast Plasmonic Control of Second Harmonic Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Davidson, Roderick B.; Yanchenko, Anna; Ziegler, Jed I.

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-fieldmore » is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.« less

Ultrafast Plasmonic Control of Second Harmonic Generation

DOE PAGES

Davidson, Roderick B.; Yanchenko, Anna; Ziegler, Jed I.; ...

2016-06-01

Efficient frequency conversion techniques are crucial to the development of plasmonic metasurfaces for information processing and signal modulation. In principle, nanoscale electric-field confinement in nonlinear materials enables higher harmonic conversion efficiencies per unit volume than those attainable in bulk materials. Here we demonstrate efficient second-harmonic generation (SHG) in a serrated nanogap plasmonic geometry that generates steep electric field gradients on a dielectric metasurface. An ultrafast control pulse is used to control plasmon-induced electric fields in a thin-film material with inversion symmetry that, without plasmonic enhancement, does not exhibit an even-order nonlinear optical response. The temporal evolution of the plasmonic near-fieldmore » is characterized with ~100 as resolution using a novel nonlinear interferometric technique. The serrated nanogap is a unique platform in which to investigate optically controlled, plasmonically enhanced harmonic generation in dielectric materials on an ultrafast time scale. Lastly, this metamaterial geometry can also be readily extended to all-optical control of other nonlinear phenomena, such as four-wave mixing and sum- and difference-frequency generation, in a wide variety of dielectric materials.« less

Ultrafast time scale X-rotation of cold atom storage qubit using Rubidium clock states

NASA Astrophysics Data System (ADS)

Song, Yunheung; Lee, Han-Gyeol; Kim, Hyosub; Jo, Hanlae; Ahn, Jaewook

2017-04-01

Ultrafast-time-scale optical interaction is a local operation on the electronic subspace of an atom, thus leaving its nuclear state intact. However, because atomic clock states are maximally entangled states of the electronic and nuclear degrees of freedom, their entire Hilbert space should be accessible only with local operations and classical communications (LOCC). Therefore, it may be possible to achieve hyperfine qubit gates only with electronic transitions. Here we show an experimental implementation of ultrafast X-rotation of atomic hyperfine qubits, in which an optical Rabi oscillation induces a geometric phase between the constituent fine-structure states, thus bringing about the X-rotation between the two ground hyperfine levels. In experiments, cold atoms in a magneto-optical trap were controlled with a femtosecond laser pulse from a Ti:sapphire laser amplifier. Absorption imaging of the as-controlled atoms initially in the ground hyperfine state manifested polarization dependence, strongly agreeing with the theory. The result indicates that single laser pulse implementations of THz clock speed qubit controls are feasible for atomic storage qubits. Samsung Science and Technology Foundation [SSTF-BA1301-12].

Quantum Femtosecond Magnetism: Phase Transition in Step with Light in a Strongly Correlated Manganese Oxide

NASA Astrophysics Data System (ADS)

Wang, Jigang

2014-03-01

Research of non-equilibrium phase transitions of strongly correlated electrons is built around addressing an outstanding challenge: how to achieve ultrafast manipulation of competing magnetic/electronic phases and reveal thermodynamically hidden orders at highly non-thermal, femtosecond timescales? Recently we reveal a new paradigm called quantum femtosecond magnetism-photoinduced femtosecond magnetic phase transitions driven by quantum spin flip fluctuations correlated with laser-excited inter-atomic coherent bonding. We demonstrate an antiferromagnetic (AFM) to ferromagnetic (FM) switching during about 100 fs laser pulses in a colossal magneto-resistive manganese oxide. Our results show a huge photoinduced femtosecond spin generation, measured by magnetic circular dichroism, with photo-excitation threshold behavior absent in the picosecond dynamics. This reveals an initial quantum coherent regime of magnetism, while the optical polarization/coherence still interacts with the spins to initiate local FM correlations that compete with the surrounding AFM matrix. Our results thus provide a framework that explores quantum non-equilibrium kinetics to drive phase transitions between exotic ground states in strongly correlated elecrons, and raise fundamental questions regarding some accepted rules, such as free energy and adiabatic potential surface. This work is in collaboration with Tianqi Li, Aaron Patz, Leonidas Mouchliadis, Jiaqiang Yan, Thomas A. Lograsso, Ilias E. Perakis. This work was supported by the National Science Foundation (contract no. DMR-1055352). Material synthesis at the Ames Laboratory was supported by the US Department of Energy-Basic Energy Sciences (contract no. DE-AC02-7CH11358).

Phosphorene quantum dot saturable absorbers for ultrafast fiber lasers

PubMed Central

Du, J.; Zhang, M.; Guo, Z.; Chen, J.; Zhu, X.; Hu, G.; Peng, P.; Zheng, Z.; Zhang, H.

2017-01-01

We fabricate ultrasmall phosphorene quantum dots (PQDs) with an average size of 2.6 ± 0.9 nm using a liquid exfoliation method involving ultrasound probe sonication followed by bath sonication. By coupling the as-prepared PQDs with microfiber evanescent light field, the PQD-based saturable absorber (SA) device exhibits ultrafast nonlinear saturable absorption property, with an optical modulation depth of 8.1% at the telecommunication band. With the integration of the all-fiber PQD-based SA, a continuous-wave passively mode-locked erbium-doped (Er-doped) laser cavity delivers stable, self-starting pulses with a pulse duration of 0.88 ps and at the cavity repetition rate of 5.47 MHz. Our results contribute to the growing body of work studying the nonlinear optical properties of ultrasmall PQDs that present new opportunities of this two-dimensional (2D) nanomaterial for future ultrafast photonic technologies. PMID:28211471

Ultra-fast dynamics in the nonlinear optical response of silver nanoprism ordered arrays.

PubMed

Sánchez-Esquivel, Héctor; Raygoza-Sanchez, Karen Y; Rangel-Rojo, Raúl; Kalinic, Boris; Michieli, Niccolò; Cesca, Tiziana; Mattei, Giovanni

2018-03-15

In this work we present the study of the ultra-fast dynamics of the nonlinear optical response of a honeycomb array of silver triangular nanoprisms, performed using a femtosecond pulsed laser tuned with the dipolar surface plasmon resonance of the nanoarray. Nonlinear absorption and refraction, and their time-dependence, were explored using the z-scan and time-resolved excite-probe techniques. Nonlinear absorption is shown to change sign with the input irradiance and the behavior was explained on the basis of a three-level model. The response time was determined to be in the picosecond regime. A technique based on a variable frequency chopper was also used in order to discriminate the thermal and electronic contributions to the nonlinearity, which were found to have opposite signs. All these findings propel the investigated nanoprism arrays as good candidates for applications in advanced ultra-fast nonlinear nanophotonic devices.

Realizing high-quality ultralarge momentum states and ultrafast topological transitions using semiconductor hyperbolic metamaterials

DOE PAGES

Campione, Salvatore; Liu, Sheng; Luk, Ting S.; ...

2015-08-05

We employ both the effective medium approximation (EMA) and Bloch theory to compare the dispersion properties of semiconductor hyperbolic metamaterials (SHMs) at mid-infrared frequencies and metallic hyperbolic metamaterials (MHMs) at visible frequencies. This analysis reveals the conditions under which the EMA can be safely applied for both MHMs and SHMs. We find that the combination of precise nanoscale layering and the longer infrared operating wavelengths puts the SHMs well within the effective medium limit and, in contrast to MHMs, allows for the attainment of very high photon momentum states. Additionally, SHMs allow for new phenomena such as ultrafast creation ofmore » the hyperbolic manifold through optical pumping. Furthermore, we examine the possibility of achieving ultrafast topological transitions through optical pumping which can photo-dope appropriately designed quantum wells on the femtosecond time scale.« less

Effect of Carrier Thermalization Dynamics on Light Emission and Amplification in Organometal Halide Perovskites.

PubMed

Chen, Kai; Barker, Alex J; Morgan, Francis L C; Halpert, Jonathan E; Hodgkiss, Justin M

2015-01-02

The remarkable rise of organometal halide perovskites as solar photovoltaic materials has been followed by promising developments in light-emitting devices, including lasers. Here we present unique insights into the processes leading to photon emission in these materials. We employ ultrafast broadband photoluminescence (PL) and transient absorption spectroscopies to directly link density dependent ultrafast charge dynamics to PL. We find that exceptionally strong PL at the band edge is preceded by thermalization of free charge carriers. Short-lived PL above the band gap is clear evidence of nonexcitonic emission from hot carriers, and ultrafast PL depolarization confirms that uncorrelated charge pairs are precursors to photon emission. Carrier thermalization has a profound effect on amplified stimulated emission at high fluence; the delayed onset of optical gain we resolve within the first 10 ps and the unusual oscillatory behavior are both consequences of the kinetic interplay between carrier thermalization and optical gain.

Ultrafast dynamics of electrons in ammonia.

PubMed

Vöhringer, Peter

2015-04-01

Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron.

Interface-induced phenomena in magnetism

DOE PAGES

Hellman, Frances; Hoffmann, Axel; Tserkovnyak, Yaroslav; ...

2017-06-05

Our article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important conceptsmore » include spin accumulation, spin currents, spin transfer torque, and spin pumping. We provide an overview for the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. Our article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes.« less

Interface-Induced Phenomena in Magnetism

PubMed Central

Hoffmann, Axel; Tserkovnyak, Yaroslav; Beach, Geoffrey S. D.; Fullerton, Eric E.; Leighton, Chris; MacDonald, Allan H.; Ralph, Daniel C.; Arena, Dario A.; Dürr, Hermann A.; Fischer, Peter; Grollier, Julie; Heremans, Joseph P.; Jungwirth, Tomas; Kimel, Alexey V.; Koopmans, Bert; Krivorotov, Ilya N.; May, Steven J.; Petford-Long, Amanda K.; Rondinelli, James M.; Samarth, Nitin; Schuller, Ivan K.; Slavin, Andrei N.; Stiles, Mark D.; Tchernyshyov, Oleg; Thiaville, André; Zink, Barry L.

2017-01-01

This article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important concepts include spin accumulation, spin currents, spin transfer torque, and spin pumping. An overview is provided to the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. The article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes. PMID:28890576

An innovative Yb-based ultrafast deep ultraviolet source for time-resolved photoemission experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Boschini, F.; Hedayat, H.; Dallera, C.

2014-12-15

Time- and angle-resolved photoemission spectroscopy is a powerful technique to study ultrafast electronic dynamics in solids. Here, an innovative optical setup based on a 100-kHz Yb laser source is presented. Exploiting non-collinear optical parametric amplification and sum-frequency generation, ultrashort pump (hν = 1.82 eV) and ultraviolet probe (hν = 6.05 eV) pulses are generated. Overall temporal and instrumental energy resolutions of, respectively, 85 fs and 50 meV are obtained. Time- and angle-resolved measurements on BiTeI semiconductor are presented to show the capabilities of the setup.

QoS support over ultrafast TDM optical networks

NASA Astrophysics Data System (ADS)

Narvaez, Paolo; Siu, Kai-Yeung; Finn, Steven G.

1999-08-01

HLAN is a promising architecture to realize Tb/s access networks based on ultra-fast optical TDM technologies. This paper presents new research results on efficient algorithms for the support of quality of service over the HLAN network architecture. In particular, we propose a new scheduling algorithm that emulates fair queuing in a distributed manner for bandwidth allocation purpose. The proposed scheduler collects information on the queue of each host on the network and then instructs each host how much data to send. Our new scheduling algorithm ensures full bandwidth utilization, while guaranteeing fairness among all hosts.

Fast responses from slowly relaxing'' liquids: A comparative study of the femtosecond dynamics of triacetin, ethylene glycol, and water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Y.J.; Castner, E.W. Jr.

1993-11-15

We have measured the ultrafast solvent relaxation of liquid ethylene glycol, triacetin, and water by means of femtosecond polarization spectroscopy, using optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy. In the viscous liquids triacetin and ethylene glycol, femtosecond relaxation processes were resolved. Not surprisingly, the femtosecond nonlinear optical response of ethylene glycol is quite similar to that of water. Using the theory of Maroncelli, Kumar, and Papazyan, we transform the pure-nuclear solvent response into a dipolar-solvation correlation function for comparison with ultrafast electron-transfer reaction rates.

Fast responses from ``slowly relaxing'' liquids: A comparative study of the femtosecond dynamics of triacetin, ethylene glycol, and water

NASA Astrophysics Data System (ADS)

Chang, Yong Joon; Castner, Edward W., Jr.

1993-11-01

We have measured the ultrafast solvent relaxation of liquid ethylene glycol, triacetin, and water by means of femtosecond polarization spectroscopy, using optical-heterodyne-detected Raman-induced Kerr-effect spectroscopy. In the viscous liquids triacetin and ethylene glycol, femtosecond relaxation processes were resolved. Not surprisingly, the femtosecond nonlinear optical response of ethylene glycol is quite similar to that of water. Using the theory of Maroncelli, Kumar, and Papazyan, we transform the pure-nuclear solvent response into a dipolar-solvation correlation function for comparison with ultrafast electron-transfer reaction rates.

Time-resolved fluorescence and ultrafast energy transfer in a zinc (hydr)oxide-graphite oxide mesoporous composite

NASA Astrophysics Data System (ADS)

Secor, Jeff; Narinesingh, Veeshan; Seredych, Mykola; Giannakoudakis, Dimitrios A.; Bandosz, Teresa; Alfano, Robert R.

2015-01-01

Ultrafast energy decay kinetics of a zinc (hydr)oxide-graphite oxide (GO) composite is studied via time-resolved fluorescence spectroscopy. The time-resolved emission is spectrally decomposed into emission regions originating from the zinc (hydr)oxide optical gap, surface, and defect states of the composite material. The radiative lifetime of deep red emission becomes an order of magnitude longer than that of GO alone while the radiative lifetime of the zinc optical gap is shortened in the composite. An energy transfer scheme from the zinc (hydr)oxide to GO is considered.

Ultrafast Optical Microscopy of Single Monolayer Molybdenum Disulfide Flakes

DOE PAGES

Seo, Minah; Yamaguchi, Hisato; Mohite, Aditya D.; ...

2016-02-15

We performed ultrafast optical microscopy on single flakes of atomically thin CVD-grown molybdenum disulfide, using non-degenerate femtosecond pump-probe spectroscopy to excite and probe carriers above and below the indirect and direct band gaps. These measurements reveal the influence of layer thickness on carrier dynamics when probing near the band gap. Furthermore, fluence-dependent measurements indicate that carrier relaxation is primarily influenced by surface-related defect and trap states after above-bandgap photoexcitation. Furthermore, the ability to probe femtosecond carrier dynamics in individual flakes can thus give much insight into light-matter interactions in these two-dimensional nanosystems.

Interferometer design and controls for pulse stacking in high power fiber lasers

NASA Astrophysics Data System (ADS)

Wilcox, Russell; Yang, Yawei; Dahlen, Dar; Xu, Yilun; Huang, Gang; Qiang, Du; Doolittle, Lawrence; Byrd, John; Leemans, Wim; Ruppe, John; Zhou, Tong; Sheikhsofla, Morteza; Nees, John; Galvanauskas, Almantas; Dawson, Jay; Chen, Diana; Pax, Paul

2017-03-01

In order to develop a design for a laser-plasma accelerator (LPA) driver, we demonstrate key technologies that enable fiber lasers to produce high energy, ultrafast pulses. These technologies must be scalable, and operate in the presence of thermal drift, acoustic noise, and other perturbations typical of an operating system. We show that coherent pulse stacking (CPS), which requires optical interferometers, can be made robust by image-relaying, multipass optical cavities, and by optical phase control schemes that sense pulse train amplitudes from each cavity. A four-stage pulse stacking system using image-relaying cavities is controlled for 14 hours using a pulse-pattern sensing algorithm. For coherent addition of simultaneous ultrafast pulses, we introduce a new scheme using diffractive optics, and show experimentally that four pulses can be added while a preserving pulse width of 128 fs.

Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region.

PubMed

Alam, M Zahirul; De Leon, Israel; Boyd, Robert W

2016-05-13

Nonlinear optical phenomena are crucial for a broad range of applications, such as microscopy, all-optical data processing, and quantum information. However, materials usually exhibit a weak optical nonlinearity even under intense coherent illumination. We report that indium tin oxide can acquire an ultrafast and large intensity-dependent refractive index in the region of the spectrum where the real part of its permittivity vanishes. We observe a change in the real part of the refractive index of 0.72 ± 0.025, corresponding to 170% of the linear refractive index. This change in refractive index is reversible with a recovery time of about 360 femtoseconds. Our results offer the possibility of designing material structures with large ultrafast nonlinearity for applications in nanophotonics. Copyright © 2016, American Association for the Advancement of Science.

Aqueye+: a new ultrafast single photon counter for optical high time resolution astrophysics

NASA Astrophysics Data System (ADS)

Zampieri, L.; Naletto, G.; Barbieri, C.; Verroi, E.; Barbieri, M.; Ceribella, G.; D'Alessandro, M.; Farisato, G.; Di Paola, A.; Zoccarato, P.

2015-05-01

Aqueye+ is a new ultrafast optical single photon counter, based on single photon avalanche photodiodes (SPAD) and a 4- fold split-pupil concept. It is a completely revisited version of its predecessor, Aqueye, successfully mounted at the 182 cm Copernicus telescope in Asiago. Here we will present the new technological features implemented on Aqueye+, namely a state of the art timing system, a dedicated and optimized optical train, a high sensitivity and high frame rate field camera and remote control, which will give Aqueye plus much superior performances with respect to its predecessor, unparalleled by any other existing fast photometer. The instrument will host also an optical vorticity module to achieve high performance astronomical coronography and a real time acquisition of atmospheric seeing unit. The present paper describes the instrument and its first performances.

Role of surface states and defects in the ultrafast nonlinear optical properties of CuS quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mary, K. A. Ann; Unnikrishnan, N. V., E-mail: nvu100@yahoo.com; Philip, Reji

2014-07-01

We report facile preparation of water dispersible CuS quantum dots (2–4 nm) and nanoparticles (5–11 nm) through a nontoxic, green, one-pot synthesis method. Optical and microstructural studies indicate the presence of surface states and defects (dislocations, stacking faults, and twins) in the quantum dots. The smaller crystallite size and quantum dot formation have significant effects on the high energy excitonic and low energy plasmonic absorption bands. Effective two-photon absorption coefficients measured using 100 fs laser pulses employing open-aperture Z-scan in the plasmonic region of 800 nm reveal that CuS quantum dots are better ultrafast optical limiters compared to CuS nanoparticles.

Nonreciprocal Transverse Photonic Spin and Magnetization-Induced Electromagnetic Spin-Orbit Coupling

PubMed Central

Levy, Miguel; Karki, Dolendra

2017-01-01

We present a formulation of electromagnetic spin-orbit coupling in magneto-optic media, and propose an alternative source of spin-orbit coupling to non-paraxial optics vortices. Our treatment puts forth a formulation of nonreciprocal transverse-spin angular-momentum-density shifts for evanescent waves in magneto-optic waveguide media. It shows that magnetization-induced electromagnetic spin-orbit coupling is possible, and that it leads to unequal spin to orbital angular momentum conversion in magneto-optic media evanescent waves in opposite propagation-directions. Generation of free-space helicoidal beams based on this conversion is shown to be spin-helicity- and magnetization-dependent. We show that transverse-spin to orbital angular momentum coupling into magneto-optic waveguide media engenders spin-helicity-dependent unidirectional propagation. This unidirectional effect produces different orbital angular momenta in opposite directions upon excitation-spin-helicity reversals. PMID:28059120

High-speed ultrafast laser machining with tertiary beam positioning (Conference Presentation)

NASA Astrophysics Data System (ADS)

Yang, Chuan; Zhang, Haibin

2017-03-01

For an industrial laser application, high process throughput and low average cost of ownership are critical to commercial success. Benefiting from high peak power, nonlinear absorption and small-achievable spot size, ultrafast lasers offer advantages of minimal heat affected zone, great taper and sidewall quality, and small via capability that exceeds the limits of their predecessors in via drilling for electronic packaging. In the past decade, ultrafast lasers have both grown in power and reduced in cost. For example, recently, disk and fiber technology have both shown stable operation in the 50W to 200W range, mostly at high repetition rate (beyond 500 kHz) that helps avoid detrimental nonlinear effects. However, to effectively and efficiently scale the throughput with the fast-growing power capability of the ultrafast lasers while keeping the beneficial laser-material interactions is very challenging, mainly because of the bottleneck imposed by the inertia-related acceleration limit and servo gain bandwidth when only stages and galvanometers are being used. On the other side, inertia-free scanning solutions like acoustic optics and electronic optical deflectors have small scan field, and therefore not suitable for large-panel processing. Our recent system developments combine stages, galvanometers, and AODs into a coordinated tertiary architecture for high bandwidth and meanwhile large field beam positioning. Synchronized three-level movements allow extremely fast local speed and continuous motion over the whole stage travel range. We present the via drilling results from such ultrafast system with up to 3MHz pulse to pulse random access, enabling high quality low cost ultrafast machining with emerging high average power laser sources.

Robust Stacking-Independent Ultrafast Charge Transfer in MoS2/WS2 Bilayers.

PubMed

Ji, Ziheng; Hong, Hao; Zhang, Jin; Zhang, Qi; Huang, Wei; Cao, Ting; Qiao, Ruixi; Liu, Can; Liang, Jing; Jin, Chuanhong; Jiao, Liying; Shi, Kebin; Meng, Sheng; Liu, Kaihui

2017-12-26

Van der Waals-coupled two-dimensional (2D) heterostructures have attracted great attention recently due to their high potential in the next-generation photodetectors and solar cells. The understanding of charge-transfer process between adjacent atomic layers is the key to design optimal devices as it directly determines the fundamental response speed and photon-electron conversion efficiency. However, general belief and theoretical studies have shown that the charge transfer behavior depends sensitively on interlayer configurations, which is difficult to control accurately, bringing great uncertainties in device designing. Here we investigate the ultrafast dynamics of interlayer charge transfer in a prototype heterostructure, the MoS 2 /WS 2 bilayer with various stacking configurations, by optical two-color ultrafast pump-probe spectroscopy. Surprisingly, we found that the charge transfer is robust against varying interlayer twist angles and interlayer coupling strength, in time scale of ∼90 fs. Our observation, together with atomic-resolved transmission electron characterization and time-dependent density functional theory simulations, reveals that the robust ultrafast charge transfer is attributed to the heterogeneous interlayer stretching/sliding, which provides additional channels for efficient charge transfer previously unknown. Our results elucidate the origin of transfer rate robustness against interlayer stacking configurations in optical devices based on 2D heterostructures, facilitating their applications in ultrafast and high-efficient optoelectronic and photovoltaic devices in the near future.

A dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled with a waveguide system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Boyun; Wang, Tao, E-mail: wangtao@hust.edu.cn; Tang, Jian

2014-10-07

We theoretically propose a dynamic and ultrafast group delay tuning mechanism in two microcavities side-coupled to a waveguide system through external optical pump beams. The optical Kerr effect modulation method is applied to improve tuning rate with response time of subpicoseconds or even femtoseconds. The group delay of an all-optical analog to electromagnetically induced transparency effect can be controlled by tuning either the frequency of photonic crystal microcavities or the propagation phase of line waveguide. Group delay is controlled between 5.88 and 70.98 ps by dynamically tuning resonant frequencies of the microcavities. Alternatively, the group delay is controlled between 1.86more » and 12.08 ps by dynamically tuning the propagation phase of line waveguide. All observed schemes are analyzed rigorously through finite-difference time-domain simulations and coupled-mode formalism. Results show a new direction toward microstructure integration optical pulse trapping and all-optical dynamical storage of light devices in optical communication and quantum information processing.« less

Radiation of a resonant medium excited by few-cycle optical pulses at superluminal velocity

NASA Astrophysics Data System (ADS)

Arkhipov, R. M.; Pakhomov, A. V.; Arkhipov, M. V.; Babushkin, I.; Tolmachev, Yu A.; Rosanov, N. N.

2017-05-01

Recent progress in generation of optical pulses of durations comparable to one optical cycle has presented great opportunities for studies of the fundamental processes in matter as well as time-resolved spectroscopy of ultrafast processes in nonlinear media. It opened up a new area of research in modern ultrafast nonlinear optics and led to appearance of the attosecond science. In parallel, a new research area related to emission from resonant media excited by superluminally propagating ultrashort bursts of electromagnetic radiation has been actively developed over the last few years. In this paper, we review our recent results on theoretical analysis of the Cherenkov-type radiation of a resonant medium excited by few-cycle optical pulses propagating at superluminal velocity. This situation can be realized when an electromagnetic pulse with a plane wavefront incidents on a straight string of resonant atoms or a spot of light rotates at very large angular frequency and excites a distant circular string of resonant dipoles. Theoretical analysis revealed some unusual and remarkable features of the Cherenkov radiation generated in this case. This radiation arises in a transient regime which leads to the occurrence of new frequencies in the radiation spectrum. Analysis of the characteristics of this radiation can be used for the study of the resonant structure properties. In addition, a nonlinear resonant medium excited at superluminal velocity can emit unipolar optical pulses, which can be important in ultrafast control of wave-packet dynamics of matter. Specifics of the few-cycle pulse-driven optical response of a resonant medium composed of linear and nonlinear oscillators is discussed.

Femtosecond manipulation of spins, charges, and ions in nanostructures, thin films, and surfaces

PubMed Central

Carbone, F.; Hengsberger, M.; Castiglioni, L.; Osterwalder, J.

2017-01-01

Modern ultrafast techniques provide new insights into the dynamics of ions, charges, and spins in photoexcited nanostructures. In this review, we describe the use of time-resolved electron-based methods to address specific questions such as the ordering properties of self-assembled nanoparticles supracrystals, the interplay between electronic and structural dynamics in surfaces and adsorbate layers, the light-induced control of collective electronic modes in nanowires and thin films, and the real-space/real-time evolution of the skyrmion lattice in topological magnets. PMID:29308416

The Evolution of Surface Symmetry in Femtosecond Laser-Induced Transient States of Matter

NASA Astrophysics Data System (ADS)

Garnett, Joy Carleen

Gallium arsenide and other III-V materials are well known for their excellent optical and electronic properties and have led to the development of high-performance photovoltaic cells1,2, photoelectrochemical water splitting3,4, and light emitting diodes (LEDs)5. Several combinations of III-V semiconductors are now being considered as potentially attractive alternatives to silicon for these applications. However, further development requires fundamental understanding of processes that govern light-matter interactions. Specifically, surface strain and ultrafast dynamics are of great interest to the optoelectronic industry. Strained semiconductor surfaces dominate the design of optoelectronics and III-V semiconductor-based LEDs. Currently, the structures of strained surfaces are well characterized with x-ray diffraction (XRD)6 and electron crystallography7-9. However, optically-induced electronic behavior at these interfaces are not fully understood. This has the been one of the stimulants for the research in this dissertation. To further explore opticallyinduced electronic behavior at strained interfaces, I have asked the following questions: 1. How does static optoelectronic behavior change as a function of strain? 2. How does surface symmetry and electronic motion change with respect to strain? 3. How do atomic bonds change as a function of strain? Another main research goal of this work is to understand ultrafast subpicosecond processes after pulsed laser excitation. The knowledge of ultrafast processes dominates the design of devices in industries that require high temporal and spectral resolution. Ultrafast atomic motion has been the major focus of subpicosecond structural dynamics. Currently, these dynamics upon photoexcitation are well characterized with experimental methods such as ultrafast x-ray diffraction (U-XRD), ultrafast electron diffraction (UED), and ultrafast electron crystallography (UEC). However, ultrafast atomic motion does not occur alone. The bonds connecting these moving atoms are also affected during this process. The correlation between structural and electronic dynamics is not well understood. To further explore correlated structural and electronic behavior upon ultrafast laser excitation, I have asked the following questions: 1. How does subpicosecond optoelectronic behavior change as a function of time after femtosecond pulse photoexcitation? 2. How does subpicosecond surface symmetry and electronic motion change with respect to time after femtosecond pulse photoexcitation? 3. How do atomic bonds change as a function of time after femtosecond pulse photoexcitation? To address these questions, I used experimental methods sensitive to both atomic motions and electronic responses: polarization-resolved second harmonic generation (PRSHG) and timeresolved, polarization-resolved second harmonic generation (TRPRSHG). The dissertation covers application of these techniques to III-V semiconductors: gallium arsenide (GaAs), gallium antimonide (GaSb), and aluminum gallium arsenide (AlGaAs). This dissertation is organized as follows. Chapter 2 presents the background of electronic band structures, ultrafast relaxation processes, and the origin of nonlinear optics from the perspectives of classical and quantum mechanics. It thus provides a framework for the static and transient nonlinear optical processes observed in III-V semiconductors under ultrafast pulse excitation. Next, Chapter 3 motivates the use of the experimental and analytical methods as applied to the experimental and theoretical studies outlined in Chapters 4 and 5. Chapter 4 is devoted to the understanding of polarization-resolved second-order nonlinear optical responses of various strained III-V semiconductor heterostructures resulting from defect-conducive growth conditions. Simplified phenomenological expressions for the polarization-resolved second harmonic generation (PRSHG) are first derived using tensor analysis. Afterwards, these expressions are used to fit experimental data. The developed formalism is tested under different conditions to gauge the fit robustness and sensitivity to mechanical and electronic changes in strained IIIV semiconductors. Along that same vein, Chapter 5 extends this analytical fit to describe ultrafast PRSHG responses of GaAs (100) as a function of transient changes in the interatomic potential within the first picosecond after photoexcitation. Finally, the dissertation concludes with Chapter 6 addressing possible directions for future work. The chapter begins with a description of studies to further test the sensitivity and robustness of the PRSHG phenomenological fit and how it can be used to characterize more classes of materials.

Dynamical current-induced ferromagnetic and antiferromagnetic resonances

NASA Astrophysics Data System (ADS)

Guimarães, F. S. M.; Lounis, S.; Costa, A. T.; Muniz, R. B.

2015-12-01

We demonstrate that ferromagnetic and antiferromagnetic excitations can be triggered by the dynamical spin accumulations induced by the bulk and surface contributions of the spin Hall effect. Due to the spin-orbit interaction, a time-dependent spin density is generated by an oscillatory electric field applied parallel to the atomic planes of Fe/W(110) multilayers. For symmetric trilayers of Fe/W/Fe in which the Fe layers are ferromagnetically coupled, we demonstrate that only the collective out-of-phase precession mode is excited, while the uniform (in-phase) mode remains silent. When they are antiferromagnetically coupled, the oscillatory electric field sets the Fe magnetizations into elliptical precession motions with opposite angular velocities. The manipulation of different collective spin-wave dynamical modes through the engineering of the multilayers and their thicknesses may be used to develop ultrafast spintronics devices. Our work provides a general framework that probes the realistic responses of materials in the time or frequency domain.

Orbit-induced localized spin angular momentum in strong focusing of optical vectorial vortex beams

NASA Astrophysics Data System (ADS)

Li, Manman; Cai, Yanan; Yan, Shaohui; Liang, Yansheng; Zhang, Peng; Yao, Baoli

2018-05-01

Light beams may carry optical spin or orbital angular momentum, or both. The spin and orbital parts manifest themselves by the ellipticity of the state of polarization and the vortex structure of phase of light beams, separately. Optical spin and orbit interaction, arising from the interaction between the polarization and the spatial structure of light beams, has attracted enormous interest recently. The optical spin-to-orbital angular momentum conversion under strong focusing is well known, while the converse process, orbital-to-spin conversion, has not been reported so far. In this paper, we predict in theory that the orbital angular momentum can induce a localized spin angular momentum in strong focusing of a spin-free azimuthal polarization vortex beam. This localized longitudinal spin of the focused field can drive the trapped particle to spin around its own axis. This investigation provides a new degree of freedom for spinning particles by using a vortex phase, which may have considerable potentials in optical spin and orbit interaction, light-beam shaping, or optical manipulation.

Femtosecond dynamics in hydrogen-bonded solvents

DOE Office of Scientific and Technical Information (OSTI.GOV)

Castner, E.W. Jr.; Chang, Y.J.

1993-09-01

We present results on the ultrafast dynamics of pure hydrogen-bonding solvents, obtained using femtosecond Fourier-transform optical-heterodyne-detected, Raman-induced Kerr effect spectroscopy. Solvent systems we have studied include the formamides, water, ethylene glycol, and acetic acid. Inertial and diffusive motions are clearly resolved. We comment on the effect that such ultrafast solvent motions have on chemical reactions in solution.

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

PubMed

Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

2012-08-28

Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis.

Experience-Related Structural Changes of Degenerated Occipital White Matter in Late-Blind Humans – A Diffusion Tensor Imaging Study

PubMed Central

Dietrich, Susanne; Hertrich, Ingo; Kumar, Vinod; Ackermann, Hermann

2015-01-01

Late-blind humans can learn to understand speech at ultra-fast syllable rates (ca. 20 syllables/s), a capability associated with hemodynamic activation of the central-visual system. Thus, the observed functional cross-modal recruitment of occipital cortex might facilitate ultra-fast speech processing in these individuals. To further elucidate the structural prerequisites of this skill, diffusion tensor imaging (DTI) was conducted in late-blind subjects differing in their capability of understanding ultra-fast speech. Fractional anisotropy (FA) was determined as a quantitative measure of the directionality of water diffusion, indicating fiber tract characteristics that might be influenced by blindness as well as the acquired perceptual skills. Analysis of the diffusion images revealed reduced FA in late-blind individuals relative to sighted controls at the level of the optic radiations at either side and the right-hemisphere dorsal thalamus (pulvinar). Moreover, late-blind subjects showed significant positive correlations between FA and the capacity of ultra-fast speech comprehension within right-hemisphere optic radiation and thalamus. Thus, experience-related structural alterations occurred in late-blind individuals within visual pathways that, presumably, are linked to higher order frontal language areas. PMID:25830371

New Aspects of Photocurrent Generation at Graphene pn Junctions Revealed by Ultrafast Optical Measurements

NASA Astrophysics Data System (ADS)

Aivazian, Grant; Sun, Dong; Jones, Aaron; Ross, Jason; Yao, Wang; Cobden, David; Xu, Xiaodong

2012-02-01

The remarkable electrical and optical properties of graphene make it a promising material for new optoelectronic applications. However, one important, but so far unexplored, property is the role of hot carriers in charge and energy transport at graphene interfaces. Here we investigate the photocurrent (PC) dynamics at a tunable graphene pn junction using ultrafast scanning PC microscopy. Pump-probe measurements show a temperature dependent relaxation time of photogenerated carriers that increases from 1.5ps at 290K to 4ps at 20K; while the amplitude of the PC is independent of the lattice temperature. These observations imply that it is hot carriers, not phonons, which dominate ultrafast energy transport. Gate dependent measurements show many interesting features such as pump induced saturation, enhancement, and sign reversal of probe generated PC. These observations reveal that the underlying PC mechanism is a combination of the thermoelectric and built-in electric field effects. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (˜500 GHz) for graphene-based photodetectors.

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface.

PubMed

Sykes, Matthew E; Stewart, Jon W; Akselrod, Gleb M; Kong, Xiang-Tian; Wang, Zhiming; Gosztola, David J; Martinson, Alex B F; Rosenmann, Daniel; Mikkelsen, Maiken H; Govorov, Alexander O; Wiederrecht, Gary P

2017-10-17

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers, which we propose arise from anisotropic electron-electron scattering within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold, whereas the quantum process of hot electron generation takes place in both components. Our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.The creation of energetic electrons through plasmon excitation has implications in optical energy conversion and ultrafast nanophotonics. Here, the authors find evidence for three subpopulations of nonthermal carriers which arise from anisotropic electron-electron scattering near the Fermi surface.

Plasmonic antennas as design elements for coherent ultrafast nanophotonics.

PubMed

Brinks, Daan; Castro-Lopez, Marta; Hildner, Richard; van Hulst, Niek F

2013-11-12

Broadband excitation of plasmons allows control of light-matter interaction with nanometric precision at femtosecond timescales. Research in the field has spiked in the past decade in an effort to turn ultrafast plasmonics into a diagnostic, microscopy, computational, and engineering tool for this novel nanometric-femtosecond regime. Despite great developments, this goal has yet to materialize. Previous work failed to provide the ability to engineer and control the ultrafast response of a plasmonic system at will, needed to fully realize the potential of ultrafast nanophotonics in physical, biological, and chemical applications. Here, we perform systematic measurements of the coherent response of plasmonic nanoantennas at femtosecond timescales and use them as building blocks in ultrafast plasmonic structures. We determine the coherent response of individual nanoantennas to femtosecond excitation. By mixing localized resonances of characterized antennas, we design coupled plasmonic structures to achieve well-defined ultrafast and phase-stable field dynamics in a predetermined nanoscale hotspot. We present two examples of the application of such structures: control of the spectral amplitude and phase of a pulse in the near field, and ultrafast switching of mutually coherent hotspots. This simple, reproducible and scalable approach transforms ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid-state physics, and quantum biology.

Probing ultrafast proton induced dynamics in transparent dielectrics

NASA Astrophysics Data System (ADS)

Taylor, M.; Coughlan, M.; Nersisyan, G.; Senje, L.; Jung, D.; Currell, F.; Riley, D.; Lewis, C. L. S.; Zepf, M.; Dromey, B.

2018-05-01

A scheme has been developed permitting the spatial and temporal characterisation of ultrafast dynamics induced by laser driven proton bursts in transparent dielectrics. Advantage is taken of the high degree of synchronicity between the proton bursts generated during laser-foil target interactions and the probing laser to provide the basis for streaking of the dynamics. Relaxation times of electrons (<10‑12 s) are measured following swift excitation across the optical band gap for various glass samples. A temporal resolution of <500 fs is achieved demonstrating that these ultrafast dynamics can be characterized on a single-shot basis.

Ultrafast laser ablation for targeted atherosclerotic plaque removal

NASA Astrophysics Data System (ADS)

Lanvin, Thomas; Conkey, Donald B.; Descloux, Laurent; Frobert, Aurelien; Valentin, Jeremy; Goy, Jean-Jacques; Cook, Stéphane; Giraud, Marie-Noelle; Psaltis, Demetri

2015-07-01

Coronary artery disease, the main cause of heart disease, develops as immune cells and lipids accumulate into plaques within the coronary arterial wall. As a plaque grows, the tissue layer (fibrous cap) separating it from the blood flow becomes thinner and increasingly susceptible to rupturing and causing a potentially lethal thrombosis. The stabilization and/or treatment of atherosclerotic plaque is required to prevent rupturing and remains an unsolved medical problem. Here we show for the first time targeted, subsurface ablation of atherosclerotic plaque using ultrafast laser pulses. Excised atherosclerotic mouse aortas were ablated with ultrafast near-infrared (NIR) laser pulses. The physical damage was characterized with histological sections of the ablated atherosclerotic arteries from six different mice. The ultrafast ablation system was integrated with optical coherence tomography (OCT) imaging for plaque-specific targeting and monitoring of the resulting ablation volume. We find that ultrafast ablation of plaque just below the surface is possible without causing damage to the fibrous cap, which indicates the potential use of ultrafast ablation for subsurface atherosclerotic plaque removal. We further demonstrate ex vivo subsurface ablation of a plaque volume through a catheter device with the high-energy ultrafast pulse delivered via hollow-core photonic crystal fiber.

Optical Control of a Nuclear Spin in Diamond

NASA Astrophysics Data System (ADS)

Levonian, David; Goldman, Michael; Degreve, Kristiaan; Choi, Soonwon; Markham, Matthew; Twitchen, Daniel; Lukin, Mikhail

2017-04-01

The nitrogen-vacancy (NV) center in diamond has emerged as a promising candidate for quantum information and quantum communication applications. The NV center's potential as a quantum register is due to the long coherence time of its spin-triplet electronic ground state, the optical addressability of its electronic transitions, and the presence of nearby ancillary nuclear spins. The NV center's electronic spin and nearby nuclear spins are most commonly manipulated using applied microwave and RF fields, but this approach would be difficult to scale up for use with an array of NV-based quantum registers. In this context, all-optical manipulation would be more scalable, technically simpler, and potentially faster. Although all-optical control of the electronic spin has been demonstrated, it is an outstanding problem for the nuclear spins. Here, we use an optical Raman scheme to implement nuclear spin-specific control of the electronic spin and coherent control of the 14N nuclear spin.

Initial Atomic Motion Immediately Following Femtosecond-Laser Excitation in Phase-Change Materials.

PubMed

Matsubara, E; Okada, S; Ichitsubo, T; Kawaguchi, T; Hirata, A; Guan, P F; Tokuda, K; Tanimura, K; Matsunaga, T; Chen, M W; Yamada, N

2016-09-23

Despite the fact that phase-change materials are widely used for data storage, no consensus exists on the unique mechanism of their ultrafast phase change and its accompanied large and rapid optical change. By using the pump-probe observation method combining a femtosecond optical laser and an x-ray free-electron laser, we substantiate experimentally that, in both GeTe and Ge_{2}Sb_{2}Te_{5} crystals, rattling motion of mainly Ge atoms takes place with keeping the off-center position just after femtosecond-optical-laser irradiation, which eventually leads to a higher symmetry or disordered state. This very initial rattling motion in the undistorted lattice can be related to instantaneous optical change due to the loss of resonant bonding that characterizes GeTe-based phase change materials. Based on the amorphous structure derived by first-principles molecular dynamics simulation, we infer a plausible ultrafast amorphization mechanism via nonmelting.

Probing ultrafast spin dynamics with high-harmonic magnetic circular dichroism spectroscopy

NASA Astrophysics Data System (ADS)

Willems, F.; Smeenk, C. T. L.; Zhavoronkov, N.; Kornilov, O.; Radu, I.; Schmidbauer, M.; Hanke, M.; von Korff Schmising, C.; Vrakking, M. J. J.; Eisebitt, S.

2015-12-01

Magnetic circular dichroism in the extreme ultraviolet (XUV) spectral range is a powerful technique for element-specific probing of magnetization in multicomponent magnetic alloys and multilayers. We combine a high-harmonic generation source with a λ /4 phase shifter to obtain circularly polarized XUV femtosecond pulses for ultrafast magnetization studies. We report on simultaneously measured resonant magnetic circular dichroism (MCD) of Co and Ni at their respective M2 ,3 edges and of Pt at its O edge, originating from interface magnetism. We present a time-resolved MCD absorption measurement of a thin magnetic Pt/Co/Pt film, showing simultaneous demagnetization of Co and Pt on a femtosecond time scale.

A new detection scheme for ultrafast 2D J-resolved spectroscopy

NASA Astrophysics Data System (ADS)

Giraudeau, Patrick; Akoka, Serge

2007-06-01

Recent ultrafast techniques enable 2D NMR spectra to be obtained in a single scan. A modification of the detection scheme involved in this technique is proposed, permitting the achievement of 2D 1H J-resolved spectra in 500 ms. The detection gradient echoes are substituted by spin echoes to obtain spectra where the coupling constants are encoded along the direct ν2 domain. The use of this new J-resolved detection block after continuous phase-encoding excitation schemes is discussed in terms of resolution and sensitivity. J-resolved spectra obtained on cinnamic acid and 3-ethyl bromopropionate are presented, revealing the expected 2D J-patterns with coupling constants as small as 2 Hz.

Nanosystems in ultrafast and superstrong fields: attosecond phenomena (Conference Presentation)

NASA Astrophysics Data System (ADS)

Stockman, Mark I.

2017-02-01

We present our latest results for a new class of phenomena in condensed matter nanooptics when a strong optical field ˜1-3 V/Å changes a solid within optical cycle [1-8]. Such a pulse drives ampere-scale currents in dielectrics and adiabatically controls their properties, including optical absorption and reflection, extreme UV absorption, and generation of high harmonics [9] in a non-perturbative manner on a 100-as temporal scale. Applied to a metal, such a pulse causes an instantaneous and, potentially, reversible change from the metallic to semimetallic properties. We will also discuss our latest theoretical results on graphene that in a strong ultrashort pulse field exhibits unique behavior [10-12]. New phenomena are predicted for buckled two-dimensional solids, silicene and germanene [13]. These are fastest phenomena in optics unfolding within half period of light. They offer potential for petahertz-bandwidth signal processing, generation of high harmonics on a nanometer spatial scale, etc. References 1. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Metallization of Nanofilms in Strong Adiabatic Electric Fields, Phys. Rev. Lett. 105, 086803-1-4 (2010). 2. M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, Predicted Ultrafast Dynamic Metallization of Dielectric Nanofilms by Strong Single-Cycle Optical Fields, Phys. Rev. Lett. 107, 086602-1-5 (2011). 3. A. Schiffrin, T. Paasch-Colberg, N. Karpowicz, V. Apalkov, D. Gerster, S. Muhlbrandt, M. Korbman, J. Reichert, M. Schultze, S. Holzner, J. V. Barth, R. Kienberger, R. Ernstorfer, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Optical-Field-Induced Current in Dielectrics, Nature 493, 70-74 (2013). 4. M. Schultze, E. M. Bothschafter, A. Sommer, S. Holzner, W. Schweinberger, M. Fiess, M. Hofstetter, R. Kienberger, V. Apalkov, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Controlling Dielectrics with the Electric Field of Light, Nature 493, 75-78 (2013). 5. V. Apalkov and M. I. Stockman, Metal Nanofilm in Strong Ultrafast Optical Fields, Phys. Rev. B 88, 245438-1-7 (2013). 6. V. Apalkov and M. I. Stockman, Theory of Dielectric Nanofilms in Strong Ultrafast Optical Fields, Phys. Rev. B 86, 165118-1-13 (2012). 7. F. Krausz and M. I. Stockman, Attosecond Metrology: From Electron Capture to Future Signal Processing, Nat. Phot. 8, 205-213 (2014). 8. O. Kwon, T. Paasch-Colberg, V. Apalkov, B.-K. Kim, J.-J. Kim, M. I. Stockman, and D. E. Kim, Semimetallization of Dielectrics in Strong Optical Fields, Sci. Rep, 6, 21272-1-9 (2016). 9. T. Higuchi, M. I. Stockman, and P. Hommelhoff, Strong-Field Perspective on High-Harmonic Radiation from Bulk Solids, Phys. Rev. Lett. 113, 213901-1-5 (2014). 10. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Wannier-Stark States of Graphene in Strong Electric Field, Phys. Rev. B 90, 085313-1-11 (2014). 11. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Graphene in Ultrafast and Superstrong Laser Fields, Phys. Rev. B 91, 0454391-8 (2015). 12. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Attosecond Strong-Field Interferometry in Graphene: Chirality, Singularity, and Berry Phase, Phys. Rev. B 93, 155434-1-7 (2016). 13. H. K. Kelardeh, V. Apalkov, and M. I. Stockman, Ultrafast Field Control of Symmetry, Reciprocity, and Reversibility in Buckled Graphene-Like Materials, Phys. Rev. B 92, 045413-1-9 (2015).

Surface Plasmon-Mediated Nanoscale Localization of Laser-Driven sub-Terahertz Spin Dynamics in Magnetic Dielectrics.

PubMed

Chekhov, Alexander L; Stognij, Alexander I; Satoh, Takuya; Murzina, Tatiana V; Razdolski, Ilya; Stupakiewicz, Andrzej

2018-05-09

We report spatial localization of the effective magnetic field generated via the inverse Faraday effect employing surface plasmon polaritons (SPPs) at Au/garnet interface. Analyzing both numerically and analytically the electric field of the SPPs at this interface, we corroborate our study with a proof-of-concept experiment showing efficient SPP-driven excitation of coherent spin precession with 0.41 THz frequency. We argue that the subdiffractional confinement of the SPP electric field enables strong spatial localization of the SPP-mediated excitation of spin dynamics. We demonstrate two orders of magnitude enhancement of the excitation efficiency at the surface plasmon resonance within a 100 nm layer of a dielectric garnet. Our findings broaden the horizons of ultrafast spin-plasmonics and open pathways toward nonthermal opto-magnetic recording on the nanoscale.

Thermal effects in an ultrafast BiB 3O 6 optical parametric oscillator at high average powers

DOE PAGES

Petersen, T.; Zuegel, J. D.; Bromage, J.

2017-08-15

An ultrafast, high-average-power, extended-cavity, femtosecond BiB 3O 6 optical parametric oscillator was constructed as a test bed for investigating the scalability of infrared parametric devices. Despite the high pulse energies achieved by this system, the reduction in slope efficiency near the maximum-available pump power prompted the investigation of thermal effects in the crystal during operation. Furthermore, the local heating effects in the crystal were used to determine the impact on both phase matching and thermal lensing to understand limitations that must be overcome to achieve microjoule-level pulse energies at high repetition rates.

Ultrafast Airy beam optical parametric oscillator

PubMed Central

Apurv Chaitanya, N.; Kumar, S. Chaitanya; Aadhi, A.; Samanta, G. K.; Ebrahim-Zadeh, M.

2016-01-01

We report on the first realization of an ultrafast Airy beam optical parametric oscillator (OPO). By introducing intracavity cubic phase modulation to the resonant Gaussian signal in a synchronously-pumped singly-resonant OPO cavity and its subsequent Fourier transformation, we have generated 2-dimensional Airy beam in the output signal across a 250 nm tuning range in the near-infrared. The generated Airy beam can be tuned continuously from 1477 to 1727 nm, providing an average power of as much as 306 mW at 1632 nm in pulses of ~23 ps duration with a spectral bandwidth of 1.7 nm. PMID:27476910

Thermal effects in an ultrafast BiB 3O 6 optical parametric oscillator at high average powers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Petersen, T.; Zuegel, J. D.; Bromage, J.

An ultrafast, high-average-power, extended-cavity, femtosecond BiB 3O 6 optical parametric oscillator was constructed as a test bed for investigating the scalability of infrared parametric devices. Despite the high pulse energies achieved by this system, the reduction in slope efficiency near the maximum-available pump power prompted the investigation of thermal effects in the crystal during operation. Furthermore, the local heating effects in the crystal were used to determine the impact on both phase matching and thermal lensing to understand limitations that must be overcome to achieve microjoule-level pulse energies at high repetition rates.

Universal spin-momentum locked optical forces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kalhor, Farid; Thundat, Thomas; Jacob, Zubin, E-mail: zjacob@purdue.edu

2016-02-08

Evanescent electromagnetic waves possess spin-momentum locking, where the direction of propagation (momentum) is locked to the inherent polarization of the wave (transverse spin). We study the optical forces arising from this universal phenomenon and show that the fundamental origin of recently reported non-trivial optical chiral forces is spin-momentum locking. For evanescent waves, we show that the direction of energy flow, the direction of decay, and the direction of spin follow a right hand rule for three different cases of total internal reflection, surface plasmon polaritons, and HE{sub 11} mode of an optical fiber. Furthermore, we explain how the recently reportedmore » phenomena of lateral optical force on chiral and achiral particles are caused by the transverse spin of the evanescent field and the spin-momentum locking phenomenon. Finally, we propose an experiment to identify the unique lateral forces arising from the transverse spin in the optical fiber and point to fundamental differences of the spin density from the well-known orbital angular momentum of light. Our work presents a unified view on spin-momentum locking and how it affects optical forces on chiral and achiral particles.« less

Time-resolved molecular imaging

NASA Astrophysics Data System (ADS)

Xu, Junliang; Blaga, Cosmin I.; Agostini, Pierre; DiMauro, Louis F.

2016-06-01

Time-resolved molecular imaging is a frontier of ultrafast optical science and physical chemistry. In this article, we review present and future key spectroscopic and microscopic techniques for ultrafast imaging of molecular dynamics and show their differences and connections. The advent of femtosecond lasers and free electron x-ray lasers bring us closer to this goal, which eventually will extend our knowledge about molecular dynamics to the attosecond time domain.

Ultrafast time-stretch imaging at 932 nm through a new highly-dispersive fiber

PubMed Central

Wei, Xiaoming; Kong, Cihang; Sy, Samuel; Ko, Ho; Tsia, Kevin K.; Wong, Kenneth K. Y.

2016-01-01

Optical glass fiber has played a key role in the development of modern optical communication and attracted the biotechnology researcher’s great attention because of its properties, such as the wide bandwidth, low attenuation and superior flexibility. For ultrafast optical imaging, particularly, it has been utilized to perform MHz time-stretch imaging with diffraction-limited resolutions, which is also known as serial time-encoded amplified microscopy (STEAM). Unfortunately, time-stretch imaging with dispersive fibers has so far mostly been demonstrated at the optical communication window of 1.5 μm due to lack of efficient dispersive optical fibers operating at the shorter wavelengths, particularly at the bio-favorable window, i.e., <1.0 μm. Through fiber-optic engineering, here we demonstrate a 7.6-MHz dual-color time-stretch optical imaging at bio-favorable wavelengths of 932 nm and 466 nm. The sensitivity at such a high speed is experimentally identified in a slow data-streaming manner. To the best of our knowledge, this is the first time that all-optical time-stretch imaging at ultrahigh speed, high sensitivity and high chirping rate (>1 ns/nm) has been demonstrated at a bio-favorable wavelength window through fiber-optic engineering. PMID:28018737

Ultrafast time-stretch imaging at 932 nm through a new highly-dispersive fiber.

PubMed

Wei, Xiaoming; Kong, Cihang; Sy, Samuel; Ko, Ho; Tsia, Kevin K; Wong, Kenneth K Y

2016-12-01

Optical glass fiber has played a key role in the development of modern optical communication and attracted the biotechnology researcher's great attention because of its properties, such as the wide bandwidth, low attenuation and superior flexibility. For ultrafast optical imaging, particularly, it has been utilized to perform MHz time-stretch imaging with diffraction-limited resolutions, which is also known as serial time-encoded amplified microscopy (STEAM). Unfortunately, time-stretch imaging with dispersive fibers has so far mostly been demonstrated at the optical communication window of 1.5 μm due to lack of efficient dispersive optical fibers operating at the shorter wavelengths, particularly at the bio-favorable window, i.e., <1.0 μm. Through fiber-optic engineering, here we demonstrate a 7.6-MHz dual-color time-stretch optical imaging at bio-favorable wavelengths of 932 nm and 466 nm. The sensitivity at such a high speed is experimentally identified in a slow data-streaming manner. To the best of our knowledge, this is the first time that all-optical time-stretch imaging at ultrahigh speed, high sensitivity and high chirping rate (>1 ns/nm) has been demonstrated at a bio-favorable wavelength window through fiber-optic engineering.

Theory of low-power ultra-broadband terahertz sideband generation in bi-layer graphene.

PubMed

Crosse, J A; Xu, Xiaodong; Sherwin, Mark S; Liu, R B

2014-09-24

In a semiconductor illuminated by a strong terahertz (THz) field, optically excited electron-hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the THz frequency. Such high-order THz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kV cm(-1)), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker THz fields. We find that a THz field of strength 1 kV cm(-1) can produce a high-sideband spectrum of about 30 THz, 100 times broader than in GaAs. The sidebands are generated despite the absence of classical collisions, with the quantum coherence of the electron-hole pairs enabling recombination. These remarkable features lower the barrier to desktop electro-optical modulation at THz frequencies, facilitating ultrafast optical communications.

Ultrafast spontaneous emission of copper-doped silicon enhanced by an optical nanocavity.

PubMed

Sumikura, Hisashi; Kuramochi, Eiichi; Taniyama, Hideaki; Notomi, Masaya

2014-05-23

Dopants in silicon (Si) have attracted attention in the fields of photonics and quantum optics. However, the optical characteristics are limited by the small spontaneous emission rate of dopants in Si. This study demonstrates a large increase in the spontaneous emission rate of copper isoelectronic centres (Cu-IECs) doped into Si photonic crystal nanocavities. In a cavity with a quality factor (Q) of ~16,000, the photoluminescence (PL) lifetime of the Cu-IECs is 1.1 ns, which is 30 times shorter than the lifetime of a sample without a cavity. The PL decay rate is increased in proportion to Q/Vc (Vc is the cavity mode volume), which indicates the Purcell effect. This is the first demonstration of a cavity-enhanced ultrafast spontaneous emission from dopants in Si, and it may lead to the development of fast and efficient Si light emitters and Si quantum optical devices based on dopants with efficient optical access.

Ultrafast spontaneous emission of copper-doped silicon enhanced by an optical nanocavity

PubMed Central

SUMIKURA, HISASHI; KURAMOCHI, EIICHI; TANIYAMA, HIDEAKI; NOTOMI, MASAYA

2014-01-01

Dopants in silicon (Si) have attracted attention in the fields of photonics and quantum optics. However, the optical characteristics are limited by the small spontaneous emission rate of dopants in Si. This study demonstrates a large increase in the spontaneous emission rate of copper isoelectronic centres (Cu-IECs) doped into Si photonic crystal nanocavities. In a cavity with a quality factor (Q) of ~16,000, the photoluminescence (PL) lifetime of the Cu-IECs is 1.1 ns, which is 30 times shorter than the lifetime of a sample without a cavity. The PL decay rate is increased in proportion to Q/Vc (Vc is the cavity mode volume), which indicates the Purcell effect. This is the first demonstration of a cavity-enhanced ultrafast spontaneous emission from dopants in Si, and it may lead to the development of fast and efficient Si light emitters and Si quantum optical devices based on dopants with efficient optical access. PMID:24853336

Fine structure and optical pumping of spins in individual semiconductor quantum dots

NASA Astrophysics Data System (ADS)

Bracker, Allan S.; Gammon, Daniel; Korenev, Vladimir L.

2008-11-01

We review spin properties of semiconductor quantum dots and their effect on optical spectra. Photoluminescence and other types of spectroscopy are used to probe neutral and charged excitons in individual quantum dots with high spectral and spatial resolution. Spectral fine structure and polarization reveal how quantum dot spins interact with each other and with their environment. By taking advantage of the selectivity of optical selection rules and spin relaxation, optical spin pumping of the ground state electron and nuclear spins is achieved. Through such mechanisms, light can be used to process spins for use as a carrier of information.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope.

PubMed

Feist, Armin; Echternkamp, Katharina E; Schauss, Jakob; Yalunin, Sergey V; Schäfer, Sascha; Ropers, Claus

2015-05-14

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven 'quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Quantum coherent optical phase modulation in an ultrafast transmission electron microscope

NASA Astrophysics Data System (ADS)

Feist, Armin; Echternkamp, Katharina E.; Schauss, Jakob; Yalunin, Sergey V.; Schäfer, Sascha; Ropers, Claus

2015-05-01

Coherent manipulation of quantum systems with light is expected to be a cornerstone of future information and communication technology, including quantum computation and cryptography. The transfer of an optical phase onto a quantum wavefunction is a defining aspect of coherent interactions and forms the basis of quantum state preparation, synchronization and metrology. Light-phase-modulated electron states near atoms and molecules are essential for the techniques of attosecond science, including the generation of extreme-ultraviolet pulses and orbital tomography. In contrast, the quantum-coherent phase-modulation of energetic free-electron beams has not been demonstrated, although it promises direct access to ultrafast imaging and spectroscopy with tailored electron pulses on the attosecond scale. Here we demonstrate the coherent quantum state manipulation of free-electron populations in an electron microscope beam. We employ the interaction of ultrashort electron pulses with optical near-fields to induce Rabi oscillations in the populations of electron momentum states, observed as a function of the optical driving field. Excellent agreement with the scaling of an equal-Rabi multilevel quantum ladder is obtained, representing the observation of a light-driven `quantum walk' coherently reshaping electron density in momentum space. We note that, after the interaction, the optically generated superposition of momentum states evolves into a train of attosecond electron pulses. Our results reveal the potential of quantum control for the precision structuring of electron densities, with possible applications ranging from ultrafast electron spectroscopy and microscopy to accelerator science and free-electron lasers.

Selective resolution of photocurrent generating pathways in transition metal dichalcogenides by ultrafast microscopy (Conference Presentation)

NASA Astrophysics Data System (ADS)

Graham, Matthew W.

2017-02-01

Presently, there exists no reliable in-situ time-resolved method that selectively isolates both the recombination and escape times relevant to photocurrent generation in the ultrafast regime. Transport based measurements lack the required time resolution, while purely optical measurement give a convoluted weighted-average of all electronic dynamics, offering no selectivity for photocurrent generating pathways. Recently, the ultrafast photocurrent (U-PC) autocorrelation method has successfully measured the rate limiting electronic relaxation processes in materials such as graphene, carbon nanotubes, and transition metal dichalcogenide (TMD) materials. Here, we unambiguously derive and experimentally confirm a generic U-PC response function by simultaneously resolving the transient absorption (TA) and U-PC response for highly-efficient (48% IQE at 0 bias) WSe2 devices and twisted bilayer graphene. Surprisingly, both optical TA and electrical U-PC responses give the same E-field-dependent electronic escape and recombination rates. These rates further accurately quantify a material's intrinsic PC generation efficiency. We demonstrate that the chirality of the incident light impacts the U-PC kinetics, suggesting such measurements directly access the ultrafast dynamics need to complex electronic physics such as the valley-Hall effect. By combining E-field dependent ultrafast photocurrent with transient absorption microscopy, we have selectively imaged the dominant kinetic bottlenecks that inhibit photocurrent production in devices made from stacked few-layer TMD materials. This provides a new methodology to intelligently select materials that intrinsically avoid recombination bottlenecks and maximize photocurrent yield.

A direct temporal domain approach for ultrafast optical signal processing and its implementation using planar lightwave circuits

NASA Astrophysics Data System (ADS)

Xia, Bing

Ultrafast optical signal processing, which shares the same fundamental principles of electrical signal processing, can realize numerous important functionalities required in both academic research and industry. Due to the extremely fast processing speed, all-optical signal processing and pulse shaping have been widely used in ultrafast telecommunication networks, photonically-assisted RFlmicro-meter waveform generation, microscopy, biophotonics, and studies on transient and nonlinear properties of atoms and molecules. In this thesis, we investigate two types of optical spectrally-periodic (SP) filters that can be fabricated on planar lightwave circuits (PLC) to perform pulse repetition rate multiplication (PRRM) and arbitrary optical waveform generation (AOWG). First, we present a direct temporal domain approach for PRRM using SP filters. We show that the repetition rate of an input pulse train can be multiplied by a factor N using an optical filter with a free spectral range that does not need to be constrained to an integer multiple of N. Furthermore, the amplitude of each individual output pulse can be manipulated separately to form an arbitrary envelope at the output by optimizing the impulse response of the filter. Next, we use lattice-form Mach-Zehnder interferometers (LF-MZI) to implement the temporal domain approach for PRRM. The simulation results show that PRRM with uniform profiles, binary-code profiles and triangular profiles can be achieved. Three silica based LF-MZIs are designed and fabricated, which incorporate multi-mode interference (MMI) couplers and phase shifters. The experimental results show that 40 GHz pulse trains with a uniform envelope pattern, a binary code pattern "1011" and a binary code pattern "1101" are generated from a 10 GHz input pulse train. Finally, we investigate 2D ring resonator arrays (RRA) for ultraf ast optical signal processing. We design 2D RRAs to generate a pair of pulse trains with different binary-code patterns simultaneously from a single pulse train at a low repetition rate. We also design 2D RRAs for AOWG using the modified direct temporal domain approach. To demonstrate the approach, we provide numerical examples to illustrate the generation of two very different waveforms (square waveform and triangular waveform) from the same hyperbolic secant input pulse train. This powerful technique based on SP filters can be very useful for ultrafast optical signal processing and pulse shaping.

Ultrafast atomic-scale visualization of acoustic phonons generated by optically excited quantum dots

PubMed Central

Vanacore, Giovanni M.; Hu, Jianbo; Liang, Wenxi; Bietti, Sergio; Sanguinetti, Stefano; Carbone, Fabrizio; Zewail, Ahmed H.

2017-01-01

Understanding the dynamics of atomic vibrations confined in quasi-zero dimensional systems is crucial from both a fundamental point-of-view and a technological perspective. Using ultrafast electron diffraction, we monitored the lattice dynamics of GaAs quantum dots—grown by Droplet Epitaxy on AlGaAs—with sub-picosecond and sub-picometer resolutions. An ultrafast laser pulse nearly resonantly excites a confined exciton, which efficiently couples to high-energy acoustic phonons through the deformation potential mechanism. The transient behavior of the measured diffraction pattern reveals the nonequilibrium phonon dynamics both within the dots and in the region surrounding them. The experimental results are interpreted within the theoretical framework of a non-Markovian decoherence, according to which the optical excitation creates a localized polaron within the dot and a travelling phonon wavepacket that leaves the dot at the speed of sound. These findings indicate that integration of a phononic emitter in opto-electronic devices based on quantum dots for controlled communication processes can be fundamentally feasible. PMID:28852685

Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2.

PubMed

Dönges, Sven A; Khatib, Omar; O'Callahan, Brian T; Atkin, Joanna M; Park, Jae Hyung; Cobden, David; Raschke, Markus B

2016-05-11

Many phase transitions in correlated matter exhibit spatial inhomogeneities with expected yet unexplored effects on the associated ultrafast dynamics. Here we demonstrate the combination of ultrafast nondegenerate pump-probe spectroscopy with far from equilibrium excitation, and scattering scanning near-field optical microscopy (s-SNOM) for ultrafast nanoimaging. In a femtosecond near-field near-IR (NIR) pump and mid-IR (MIR) probe study, we investigate the photoinduced insulator-to-metal (IMT) transition in nominally homogeneous VO2 microcrystals. With pump fluences as high as 5 mJ/cm(2), we can reach three distinct excitation regimes. We observe a spatial heterogeneity on ∼50-100 nm length scales in the fluence-dependent IMT dynamics ranging from <100 fs to ∼1 ps. These results suggest a high sensitivity of the IMT with respect to small local variations in strain, doping, or defects that are difficult to discern microscopically. We provide a perspective with the distinct requirements and considerations of ultrafast spatiotemporal nanoimaging of phase transitions in quantum materials.

Self-phase modulation enabled, wavelength-tunable ultrafast fiber laser sources: an energy scalable approach.

PubMed

Liu, Wei; Li, Chen; Zhang, Zhigang; Kärtner, Franz X; Chang, Guoqing

2016-07-11

We propose and demonstrate a new approach to implement a wavelength-tunable ultrafast fiber laser source suitable for multiphoton microscopy. We employ fiber-optic nonlinearities to broaden a narrowband optical spectrum generated by an Yb-fiber laser system and then use optical bandpass filters to select the leftmost or rightmost spectral lobes from the broadened spectrum. Detailed numerical modeling shows that self-phase modulation dominates the spectral broadening, self-steepening tends to blue shift the broadened spectrum, and stimulated Raman scattering is minimal. We also find that optical wave breaking caused by fiber dispersion slows down the shift of the leftmost/rightmost spectral lobes and therefore limits the wavelength tuning range of the filtered spectra. We show both numerically and experimentally that shortening the fiber used for spectral broadening while increasing the input pulse energy can overcome this dispersion-induced limitation; as a result, the filtered spectral lobes have higher power, constituting a powerful and practical approach for energy scaling the resulting femtosecond sources. We use two commercially available photonic crystal fibers to verify the simulation results. More specific, use of 20-mm fiber NL-1050-ZERO-2 enables us to implement an Yb-fiber laser based ultrafast source, delivering femtosecond (70-120 fs) pulses tunable from 825 nm to 1210 nm with >1 nJ pulse energy.

High-yield, ultrafast, surface plasmon-enhanced, Au nanorod optical field electron emitter arrays.

PubMed

Hobbs, Richard G; Yang, Yujia; Fallahi, Arya; Keathley, Philip D; De Leo, Eva; Kärtner, Franz X; Graves, William S; Berggren, Karl K

2014-11-25

Here we demonstrate the design, fabrication, and characterization of ultrafast, surface-plasmon enhanced Au nanorod optical field emitter arrays. We present a quantitative study of electron emission from Au nanorod arrays fabricated by high-resolution electron-beam lithography and excited by 35 fs pulses of 800 nm light. We present accurate models for both the optical field enhancement of Au nanorods within high-density arrays, and electron emission from those nanorods. We have also studied the effects of surface plasmon damping induced by metallic interface layers at the substrate/nanorod interface on near-field enhancement and electron emission. We have identified the peak optical field at which the electron emission mechanism transitions from a 3-photon absorption mechanism to strong-field tunneling emission. Moreover, we have investigated the effects of nanorod array density on nanorod charge yield, including measurement of space-charge effects. The Au nanorod photocathodes presented in this work display 100-1000 times higher conversion efficiency relative to previously reported UV triggered emission from planar Au photocathodes. Consequently, the Au nanorod arrays triggered by ultrafast pulses of 800 nm light in this work may outperform equivalent UV-triggered Au photocathodes, while also offering nanostructuring of the electron pulse produced from such a cathode, which is of interest for X-ray free-electron laser (XFEL) development where nanostructured electron pulses may facilitate more efficient and brighter XFEL radiation.

All-optical control of long-lived nuclear spins in rare-earth doped nanoparticles.

PubMed

Serrano, D; Karlsson, J; Fossati, A; Ferrier, A; Goldner, P

2018-05-29

Nanoscale systems that coherently couple to light and possess spins offer key capabilities for quantum technologies. However, an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. Here, we report optically controlled nuclear spins with long coherence lifetimes (T 2 ) in rare-earth-doped nanoparticles. We detect spins echoes and measure a spin coherence lifetime of 2.9 ± 0.3 ms at 5 K under an external magnetic field of 9 mT, a T 2 value comparable to those obtained in bulk rare-earth crystals. Moreover, we achieve spin T 2 extension using all-optical spin dynamical decoupling and observe high fidelity between excitation and echo phases. Rare-earth-doped nanoparticles are thus the only nano-material in which optically controlled spins with millisecond coherence lifetimes have been reported. These results open the way to providing quantum light-atom-spin interfaces with long storage time within hybrid architectures.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses

NASA Astrophysics Data System (ADS)

Wong-Campos, J. D.; Moses, S. A.; Johnson, K. G.; Monroe, C.

2017-12-01

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ˜20 ps duration, and demonstrate an entangled Bell state with (76 ±1 )% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

Demonstration of Two-Atom Entanglement with Ultrafast Optical Pulses.

PubMed

Wong-Campos, J D; Moses, S A; Johnson, K G; Monroe, C

2017-12-08

We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just ten pulses, each of ∼20  ps duration, and demonstrate an entangled Bell state with (76±1)% fidelity. These results pave the way for entanglement operations within a large collection of qubits by exciting only local modes of motion.

Solution processable and optically switchable 1D photonic structures.

PubMed

Paternò, Giuseppe M; Iseppon, Chiara; D'Altri, Alessia; Fasanotti, Carlo; Merati, Giulia; Randi, Mattia; Desii, Andrea; Pogna, Eva A A; Viola, Daniele; Cerullo, Giulio; Scotognella, Francesco; Kriegel, Ilka

2018-02-23

We report the first demonstration of a solution processable, optically switchable 1D photonic crystal which incorporates phototunable doped metal oxide nanocrystals. The resulting device structure shows a dual optical response with the photonic bandgap covering the visible spectral range and the plasmon resonance of the doped metal oxide the near infrared. By means of a facile photodoping process, we tuned the plasmonic response and switched effectively the optical properties of the photonic crystal, translating the effect from the near infrared to the visible. The ultrafast bandgap pumping induces a signal change in the region of the photonic stopband, with recovery times of several picoseconds, providing a step toward the ultrafast optical switching. Optical modeling uncovers the importance of a complete modeling of the variations of the dielectric function of the photodoped material, including the high frequency region of the Drude response which is responsible for the strong switching in the visible after photodoping. Our device configuration offers unprecedented tunability due to flexibility in device design, covering a wavelength range from the visible to the near infrared. Our findings indicate a new protocol to modify the optical response of photonic devices by optical triggers only.

Time-resolved x-ray absorption spectroscopy: Watching atoms dance

NASA Astrophysics Data System (ADS)

Milne, Chris J.; Pham, Van-Thai; Gawelda, Wojciech; van der Veen, Renske M.; El Nahhas, Amal; Johnson, Steven L.; Beaud, Paul; Ingold, Gerhard; Lima, Frederico; Vithanage, Dimali A.; Benfatto, Maurizio; Grolimund, Daniel; Borca, Camelia; Kaiser, Maik; Hauser, Andreas; Abela, Rafael; Bressler, Christian; Chergui, Majed

2009-11-01

The introduction of pump-probe techniques to the field of x-ray absorption spectroscopy (XAS) has allowed the monitoring of both structural and electronic dynamics of disordered systems in the condensed phase with unprecedented accuracy, both in time and in space. We present results on the electronically excited high-spin state structure of an Fe(II) molecular species, [FeII(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 Å. In addition an analysis technique using the reduced χ2 goodness of fit between FEFF EXAFS simulations and the experimental transient absorption signal in energy space has been successfully tested as a function of excited state population and chemical shift, demonstrating its applicability in situations where the fractional excited state population cannot be determined through other measurements. Finally by using a novel ultrafast hard x-ray 'slicing' source the question of how the molecule relaxes after optical excitation has been successfully resolved using femtosecond XANES.

Ultrafast Imaging of Chiral Surface Plasmon by Photoemission Electron Microscopy

NASA Astrophysics Data System (ADS)

Dai, Yanan; Dabrowski, Maciej; Petek, Hrvoje

We employ Time-Resolved Photoemission Electron Microscopy (TR-PEEM) to study surface plasmon polariton (SPP) wave packet dynamics launched by tunable (VIS-UV) femtosecond pulses of various linear and circular polarizations. The plasmonic structures are micron size single-crystalline Ag islands grown in situ on Si surfaces and characterized by Low Energy Electron Microscopy (LEEM). The local fields of plasmonic modes enhance two and three photon photoemission (2PP and 3PP) at the regions of strong field enhancement. Imaging of the photoemission signal with PEEM electron optics thus images the plasmonic fields excited in the samples. The observed PEEM images with left and right circularly polarized light show chiral images, which is a consequence of the transverse spin momentum of surface plasmon. By changing incident light polarization, the plasmon interference pattern shifts with light ellipticity indicating a polarization dependent excitation phase of SPP. In addition, interferometric-time resolved measurements record the asymmetric SPP wave packet motion in order to characterize the dynamical properties of chiral SPP wave packets.

Pure-quartic solitons

PubMed Central

Blanco-Redondo, Andrea; Martijn, de Sterke C.; Sipe, J.E.; Krauss, Thomas F.; Eggleton, Benjamin J.; Husko, Chad

2016-01-01

Temporal optical solitons have been the subject of intense research due to their intriguing physics and applications in ultrafast optics and supercontinuum generation. Conventional bright optical solitons result from the interaction of anomalous group-velocity dispersion and self-phase modulation. Here we experimentally demonstrate a class of bright soliton arising purely from the interaction of negative fourth-order dispersion and self-phase modulation, which can occur even for normal group-velocity dispersion. We provide experimental and numerical evidence of shape-preserving propagation and flat temporal phase for the fundamental pure-quartic soliton and periodically modulated propagation for the higher-order pure-quartic solitons. We derive the approximate shape of the fundamental pure-quartic soliton and discover that is surprisingly Gaussian, exhibiting excellent agreement with our experimental observations. Our discovery, enabled by precise dispersion engineering, could find applications in communications, frequency combs and ultrafast lasers. PMID:26822758

Nuclear spin nanomagnet in an optically excited quantum dot.

PubMed

Korenev, V L

2007-12-21

Linearly polarized light tuned slightly below the optical transition of the negatively charged exciton (trion) in a single quantum dot causes the spontaneous nuclear spin polarization (self-polarization) at a level close to 100%. The effective magnetic field of spin-polarized nuclei shifts the optical transition energy close to resonance with photon energy. The resonantly enhanced Overhauser effect sustains the stability of the nuclear self-polarization even in the absence of spin polarization of the quantum dot electron. As a result the optically selected single quantum dot represents a tiny magnet with the ferromagnetic ordering of nuclear spins-the nuclear spin nanomagnet.

Cavity-Enhanced Optical Readout of a Single Solid-State Spin

NASA Astrophysics Data System (ADS)

Sun, Shuo; Kim, Hyochul; Solomon, Glenn S.; Waks, Edo

2018-05-01

We demonstrate optical readout of a single spin using cavity quantum electrodynamics. The spin is based on a single trapped electron in a quantum dot that has a poor branching ratio of 0.43. Selectively coupling one of the optical transitions of the quantum dot to the cavity mode results in a spin-dependent cavity reflectivity that enables spin readout by monitoring the reflected intensity of an incident optical field. Using this approach, we demonstrate spin-readout fidelity of 0.61. Achieving this fidelity using resonance fluorescence from a bare dot would require 43 times improvement in photon collection efficiency.

Photodrive of magnetic bubbles via magnetoelastic waves

PubMed Central

Ogawa, Naoki; Koshibae, Wataru; Beekman, Aron Jonathan; Nagaosa, Naoto; Kubota, Masashi; Kawasaki, Masashi; Tokura, Yoshinori

2015-01-01

Precise control of magnetic domain walls continues to be a central topic in the field of spintronics to boost infotech, logic, and memory applications. One way is to drive the domain wall by current in metals. In insulators, the incoherent flow of phonons and magnons induced by the temperature gradient can carry the spins, i.e., spin Seebeck effect, but the spatial and time dependence is difficult to control. Here, we report that coherent phonons hybridized with spin waves, magnetoelastic waves, can drive magnetic bubble domains, or curved domain walls, in an iron garnet, which are excited by ultrafast laser pulses at a nonabsorbing photon energy. These magnetoelastic waves were imaged by time-resolved Faraday microscopy, and the resultant spin transfer force was evaluated to be larger for domain walls with steeper curvature. This will pave a path for the rapid spatiotemporal control of magnetic textures in insulating magnets. PMID:26150487

Photodrive of magnetic bubbles via magnetoelastic waves.

PubMed

Ogawa, Naoki; Koshibae, Wataru; Beekman, Aron Jonathan; Nagaosa, Naoto; Kubota, Masashi; Kawasaki, Masashi; Tokura, Yoshinori

2015-07-21

Precise control of magnetic domain walls continues to be a central topic in the field of spintronics to boost infotech, logic, and memory applications. One way is to drive the domain wall by current in metals. In insulators, the incoherent flow of phonons and magnons induced by the temperature gradient can carry the spins, i.e., spin Seebeck effect, but the spatial and time dependence is difficult to control. Here, we report that coherent phonons hybridized with spin waves, magnetoelastic waves, can drive magnetic bubble domains, or curved domain walls, in an iron garnet, which are excited by ultrafast laser pulses at a nonabsorbing photon energy. These magnetoelastic waves were imaged by time-resolved Faraday microscopy, and the resultant spin transfer force was evaluated to be larger for domain walls with steeper curvature. This will pave a path for the rapid spatiotemporal control of magnetic textures in insulating magnets.

Vibronic coupling in the excited-states of carotenoids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

2016-01-01

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Vibronic coupling in the excited-states of carotenoids

DOE Office of Scientific and Technical Information (OSTI.GOV)

Miki, Takeshi; Buckup, Tiago; Krause, Marie S.

The ultrafast femtochemistry of carotenoids is governed by the interaction between electronic excited states, which has been explained by the relaxation dynamics within a few hundred femtoseconds from the lowest optically allowed excited state S 2to the optically dark state S 1.

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE PAGES

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

2017-07-01

Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the paritymore » breaking geometry change thus revealing the enantiomer asymmetry.« less

Photoinduced molecular chirality probed by ultrafast resonant X-ray spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rouxel, Jérémy R.; Kowalewski, Markus; Mukamel, Shaul

Recently developed circularly polarized X-ray light sources can probe the ultrafast chiral electronic and nuclear dynamics through spatially localized resonant core transitions. Here, we present simulations of time-resolved circular dichroism signals given by the difference of left and right circularly polarized X-ray probe transmission following an excitation by a circularly polarized optical pump with the variable time delay. Application is made to formamide which is achiral in the ground state and assumes two chiral geometries upon optical excitation to the first valence excited state. Probes resonant with various K-edges (C, N, and O) provide different local windows onto the paritymore » breaking geometry change thus revealing the enantiomer asymmetry.« less

Demonstration of the spin solar cell and spin photodiode effect

PubMed Central

Endres, B.; Ciorga, M.; Schmid, M.; Utz, M.; Bougeard, D.; Weiss, D.; Bayreuther, G.; Back, C.H.

2013-01-01

Spin injection and extraction are at the core of semiconductor spintronics. Electrical injection is one method of choice for the creation of a sizeable spin polarization in a semiconductor, requiring especially tailored tunnel or Schottky barriers. Alternatively, optical orientation can be used to generate spins in semiconductors with significant spin-orbit interaction, if optical selection rules are obeyed, typically by using circularly polarized light at a well-defined wavelength. Here we introduce a novel concept for spin injection/extraction that combines the principle of a solar cell with the creation of spin accumulation. We demonstrate that efficient optical spin injection can be achieved with unpolarized light by illuminating a p-n junction where the p-type region consists of a ferromagnet. The discovered mechanism opens the window for the optical generation of a sizeable spin accumulation also in semiconductors without direct band gap such as Si or Ge. PMID:23820766

Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics

DOE PAGES

Zhong, Ding; Seyler, Kyle L.; Linpeng, Xiayu; ...

2017-05-31

The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. We create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI 3 and a monolayer of WSe 2. We observe unprecedented control of the spin and valley pseudospin in WSe 2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe 2 valley splitting and polarization via flipping of the CrI 3 magnetization. The WSe2 photoluminescence intensity strongly depends onmore » the relative alignment between photoexcited spins in WSe 2 and the CrI 3 magnetization, because of ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure.« less

Improper magnetic ferroelectricity of nearly pure electronic nature in helicoidal spiral CaMn7O12

NASA Astrophysics Data System (ADS)

Lim, Jin Soo; Saldana-Greco, Diomedes; Rappe, Andrew M.

2018-01-01

Helicoidal magnetic order breaks inversion symmetry in quadruple perovskite CaMn7O12 , generating one of the largest spin-induced ferroelectric polarizations measured to date. Here, the microscopic origin of the polarization, including exchange interactions, coupling to the spin helicity, and charge density redistribution, is explored via first-principles calculations. The B -site Mn4 + (Mn3) spin adopts a noncentrosymmetric configuration, stabilized not only by spin-orbit coupling (SOC), but also by the fully anisotropic Hubbard J parameter in the absence of SOC, to break inversion symmetry and generate polarization. Berry phase computed polarization (Pelec=2169 μ C /m2 ) exhibits nearly pure electronic behavior, with negligible Mn displacements (≈0.7 m Å ). Orbital-resolved density of states shows that p -d orbital mixing is microscopically driven by nonrelativistic exchange striction within the commensurate ionic structure. Persistent electronic polarization induced by helical spin order in the nearly inversion-symmetric ionic crystal lattice suggests opportunities for ultrafast magnetoelectric response.

Van der Waals engineering of ferromagnetic semiconductor heterostructures for spin and valleytronics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhong, Ding; Seyler, Kyle L.; Linpeng, Xiayu

The integration of magnetic material with semiconductors has been fertile ground for fundamental science as well as of great practical interest toward the seamless integration of information processing and storage. We create van der Waals heterostructures formed by an ultrathin ferromagnetic semiconductor CrI 3 and a monolayer of WSe 2. We observe unprecedented control of the spin and valley pseudospin in WSe 2, where we detect a large magnetic exchange field of nearly 13 T and rapid switching of the WSe 2 valley splitting and polarization via flipping of the CrI 3 magnetization. The WSe2 photoluminescence intensity strongly depends onmore » the relative alignment between photoexcited spins in WSe 2 and the CrI 3 magnetization, because of ultrafast spin-dependent charge hopping across the heterostructure interface. The photoluminescence detection of valley pseudospin provides a simple and sensitive method to probe the intriguing domain dynamics in the ultrathin magnet, as well as the rich spin interactions within the heterostructure.« less

Selective excitation enables assignment of proton resonances and (1)H-(1)H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy.

PubMed

Zhang, Rongchun; Ramamoorthy, Ayyalusamy

2015-07-21

Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of (1)H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as (13)C or (15)N. In this method, after the initial preparation of proton magnetization and cross-polarization to (13)C nuclei, transverse magnetization of desired (13)C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferred to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific (13)C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of (1)H-(1)H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids.

Ultrafast far-infrared studies of vanadates &mdash Multiple routes for an insulator to metal transition

NASA Astrophysics Data System (ADS)

Liu, Mengkun

The metal insulator transition in vanadates has been studied for decades and yet new discoveries still spring up revealing new physics, especially among two of the most studied members: Vanadium sesquioxide (V20 3) and Vanadium dioxide (VO2). Although subtleties abound, both of the materials have first order insulator to metal phase transitions that are considered to be related to strong electron-electron (e-e) correlation. Further, ultrafast spectroscopy of strongly correlated materials has generated great interest in the field given the potential to dynamically distinguish the difference between electronic (spin) response versus lattice responses due to the associated characteristic energy and time scales. In this thesis, I mainly focus on utilizing ultrafast optical and THz spectroscopy to study phase transition dynamics in high quality V20 3 and VO2 thin films epitaxially grown on different substrates. The main findings of the thesis are: (1) Despite the fact that the insulator to metal transition (IMT) in V203 is electron-correlation driven, lattice distortion plays an important role. Coherent oscillations in the far-infrared conductivity are observed resulting from coherent acoustic phonon modulation of the bandwidth W. The same order of lattice distortion induces less of an effect on the electron transport in VO2 in comparison to V203. This is directly related to the difference in latent heat of the phase transitions in VO2 and V203. (2) It is possible for the IMT to occur with very little structural change in epitaxial strained VO2 films, like in the case of Cr doped or strained V203. However, in V02, this necessitates a large strain which is only possible by clamping to a substrate with larger c axis parameter through epitaxial growth. This is demonstrated for VO 2 films on TiO2 substrates. (3) Initiating an ultrafast photo-induced insulator-to-metal transition (IMT) is not only possible with above bandgap excitation, but also possible with high-field far-infrared excitation. With the help of the field enhancement in metamaterial split ring resonator gaps, we obtain picosecond THz electric field transients of several MV/cm which is sufficient to drive the insulator to metal transition in V02.

Broadly tunable ultrafast pump-probe system operating at multi-kHz repetition rate

NASA Astrophysics Data System (ADS)

Grupp, Alexander; Budweg, Arne; Fischer, Marco P.; Allerbeck, Jonas; Soavi, Giancarlo; Leitenstorfer, Alfred; Brida, Daniele

2018-01-01

Femtosecond systems based on ytterbium as active medium are ideal for driving ultrafast optical parametric amplifiers in a broad frequency range. The excellent stability of the source and the repetition rate tunable to up to hundreds of kHz allow for the implementation of an advanced two-color pump probe setup with the capability to achieve excellent signal-to-noise performances with sub-10 fs temporal resolution.

Practical method for transversely measuring the spin polarization of optically pumped alkali atoms

NASA Astrophysics Data System (ADS)

Ding, Zhichao; Yuan, Jie; Long, Xingwu

2018-06-01

A practical method to measure the spin polarization of optically pumped alkali atoms is demonstrated. In order to realize transverse measurement, the transverse spin component of spin-polarized alkali atoms is created by a rotating exciting magnetic field, and detected using the optical rotation of a near-resonant probe beam for realizing a high detection sensitivity. The dependency of the optical rotation on the spin polarization of 133Cs atoms is derived theoretically and verified experimentally. By changing the direction of the rotating magnetic field, we realize the transverse measurement of the spin polarization of 133Cs atoms in either ground-state hyperfine level.

From supersonic shear wave imaging to full-field optical coherence shear wave elastography

NASA Astrophysics Data System (ADS)

Nahas, Amir; Tanter, Mickaël; Nguyen, Thu-Mai; Chassot, Jean-Marie; Fink, Mathias; Claude Boccara, A.

2013-12-01

Elasticity maps of tissue have proved to be particularly useful in providing complementary contrast to ultrasonic imaging, e.g., for cancer diagnosis at the millimeter scale. Optical coherence tomography (OCT) offers an endogenous contrast based on singly backscattered optical waves. Adding complementary contrast to OCT images by recording elasticity maps could also be valuable in improving OCT-based diagnosis at the microscopic scale. Static elastography has been successfully coupled with full-field OCT (FF-OCT) in order to realize both micrometer-scale sectioning and elasticity maps. Nevertheless, static elastography presents a number of drawbacks, mainly when stiffness quantification is required. Here, we describe the combination of two methods: transient elastography, based on speed measurements of shear waves induced by ultrasonic radiation forces, and FF-OCT, an en face OCT approach using an incoherent light source. The use of an ultrafast ultrasonic scanner and an ultrafast camera working at 10,000 to 30,000 images/s made it possible to follow shear wave propagation with both modalities. As expected, FF-OCT is found to be much more sensitive than ultrafast ultrasound to tiny shear vibrations (a few nanometers and micrometers, respectively). Stiffness assessed in gel phantoms and an ex vivo rat brain by FF-OCT is found to be in good agreement with ultrasound shear wave elastography.

Ultrafast electron-lattice coupling dynamics in VO2 and V2O3 thin films

NASA Astrophysics Data System (ADS)

Abreu, Elsa; Gilbert Corder, Stephanie N.; Yun, Sun Jin; Wang, Siming; Ramírez, Juan Gabriel; West, Kevin; Zhang, Jingdi; Kittiwatanakul, Salinporn; Schuller, Ivan K.; Lu, Jiwei; Wolf, Stuart A.; Kim, Hyun-Tak; Liu, Mengkun; Averitt, Richard D.

2017-09-01

Ultrafast optical pump-optical probe and optical pump-terahertz probe spectroscopy were performed on vanadium dioxide (VO2) and vanadium sesquioxide (V2O3 ) thin films over a wide temperature range. A comparison of the experimental data from these two different techniques and two different vanadium oxides, in particular a comparison of the spectral weight oscillations generated by the photoinduced longitudinal acoustic modulation, reveals the strong electron-phonon coupling that exists in both materials. The low-energy Drude response of V2O3 appears more amenable than VO2 to ultrafast strain control. Additionally, our results provide a measurement of the temperature dependence of the sound velocity in both systems, revealing a four- to fivefold increase in VO2 and a three- to fivefold increase in V2O3 across the insulator-to-metal phase transition. Our data also confirm observations of strong damping and phonon anharmonicity in the metallic phase of VO2, and suggest that a similar phenomenon might be at play in the metallic phase of V2O3 . More generally, our simple table-top approach provides relevant and detailed information about dynamical lattice properties of vanadium oxides, paving the way to similar studies in other complex materials.

Giant spin Hall angle from topological insulator BixSe(1 - x) thin films

NASA Astrophysics Data System (ADS)

Dc, Mahendra; Jamali, Mahdi; Chen, Junyang; Hickey, Danielle; Zhang, Delin; Zhao, Zhengyang; Li, Hongshi; Quarterman, Patrick; Lv, Yang; Mkhyon, Andre; Wang, Jian-Ping

Investigation on the spin-orbit torque (SOT) from large spin-orbit coupling materials has been attracting interest because of its low power switching of the magnetization and ultra-fast driving of the domain wall motion that can be used in future spin based memory and logic devices. We investigated SOT from topological insulator BixSe(1 - x) thin film in BixSe(1 - x) /CoFeB heterostructure by using the dc planar Hall method, where BixSe(1 - x) thin films were prepared by a unique industry-compatible deposition process. The angle dependent Hall resistance was measured in the presence of a rotating external in-plane magnetic field at bipolar currents. The spin Hall angle (SHA) from this BixSe(1 - x) thin film was found to be as large as 22.41, which is the largest ever reported at room temperature (RT). The giant SHA and large spin Hall conductivity (SHC) make this BixSe(1 - x) thin film a very strong candidate as an SOT generator in SOT based memory and logic devices.

High-Responsivity Graphene-Boron Nitride Photodetector and Autocorrelator in a Silicon Photonic Integrated Circuit.

PubMed

Shiue, Ren-Jye; Gao, Yuanda; Wang, Yifei; Peng, Cheng; Robertson, Alexander D; Efetov, Dmitri K; Assefa, Solomon; Koppens, Frank H L; Hone, James; Englund, Dirk

2015-11-11

Graphene and other two-dimensional (2D) materials have emerged as promising materials for broadband and ultrafast photodetection and optical modulation. These optoelectronic capabilities can augment complementary metal-oxide-semiconductor (CMOS) devices for high-speed and low-power optical interconnects. Here, we demonstrate an on-chip ultrafast photodetector based on a two-dimensional heterostructure consisting of high-quality graphene encapsulated in hexagonal boron nitride. Coupled to the optical mode of a silicon waveguide, this 2D heterostructure-based photodetector exhibits a maximum responsivity of 0.36 A/W and high-speed operation with a 3 dB cutoff at 42 GHz. From photocurrent measurements as a function of the top-gate and source-drain voltages, we conclude that the photoresponse is consistent with hot electron mediated effects. At moderate peak powers above 50 mW, we observe a saturating photocurrent consistent with the mechanisms of electron-phonon supercollision cooling. This nonlinear photoresponse enables optical on-chip autocorrelation measurements with picosecond-scale timing resolution and exceptionally low peak powers.

Single-shot measurement of phase and amplitude by using a heterodyne time-lens system and ultrafast digital time-holography

NASA Astrophysics Data System (ADS)

Tikan, Alexey; Bielawski, Serge; Szwaj, Christophe; Randoux, Stéphane; Suret, Pierre

2018-04-01

Temporal imaging systems are outstanding tools for single-shot observation of optical signals that have irregular and ultrafast dynamics. They allow long time windows to be recorded with femtosecond resolution, and do not rely on complex algorithms. However, simultaneous recording of amplitude and phase remains an open challenge for these systems. Here, we present a new heterodyne time-lens arrangement that efficiently records both the amplitude and phase of complex and random signals over large temporal windows (tens of picoseconds). Phase and time are encoded onto the two spatial dimensions of a camera. We implement this phase-sensitive time-lens system in two configurations: a time microscope and a digital temporal-holography device that enables single-shot measurement with a temporal resolution of 80 fs. We demonstrate direct application of our heterodyne time-lens to turbulent-like optical fields and optical rogue waves generated from nonlinear propagation of partially coherent waves inside optical fibres.

Ultrafast acousto-plasmonics in gold nanoparticle superlattices

NASA Astrophysics Data System (ADS)

Ruello, P.; Ayouch, A.; Vaudel, G.; Pezeril, T.; Delorme, N.; Sato, S.; Kimura, K.; Gusev, V. E.

2015-11-01

We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticle superlattices (NPSs). The experiments have been performed with an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow us to estimate first the fundamental mechanical parameters such as the collective elastic response (sound velocity) of the NPS and the nanocontact elastic stiffness. Furthermore, it appears that the light-induced coherent acoustic-phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly four times the optical skin depth in gold. The modeling of the transient optical reflectivity indicates that the mechanism of phonons generation is achieved through ultrafast heating of the NPS assisted by light excitation of the volume plasmon polariton. Based on these results, we demonstrate that it is possible to map the photon-electron-phonon interaction in subwavelength nanostructures which, in particular, provides insights on the fundamental properties of these nanometamaterials.

Ultrafast nonlinear optofluidics in selectively liquid-filled photonic crystal fibers.

PubMed

Vieweg, M; Gissibl, T; Pricking, S; Kuhlmey, B T; Wu, D C; Eggleton, B J; Giessen, H

2010-11-22

Selective filling of photonic crystal fibers with different media enables a plethora of possibilities in linear and nonlinear optics. Using two-photon direct-laser writing we demonstrate full flexibility of individual closing of holes and subsequent filling of photonic crystal fibers with highly nonlinear liquids. We experimentally demonstrate solitonic supercontinuum generation over 600 nm bandwidth using a compact femtosecond oscillator as pump source. Encapsulating our fibers at the ends we realize a compact ultrafast nonlinear optofluidic device. Our work is fundamentally important to the field of nonlinear optics as it provides a new platform for investigations of spatio-temporal nonlinear effects and underpins new applications in sensing and communications. Selective filling of different linear and nonlinear liquids, metals, gases, gain media, and liquid crystals into photonic crystal fibers will be the basis of new reconfigurable and versatile optical fiber devices with unprecedented performance. Control over both temporal and spatial dispersion as well as linear and nonlinear coupling will lead to the generation of spatial-temporal solitons, so-called optical bullets.

Fabrication of semiconductor-polymer compound nonlinear photonic crystal slab with highly uniform infiltration based on nano-imprint lithography technique.

PubMed

Qin, Fei; Meng, Zi-Ming; Zhong, Xiao-Lan; Liu, Ye; Li, Zhi-Yuan

2012-06-04

We present a versatile technique based on nano-imprint lithography to fabricate high-quality semiconductor-polymer compound nonlinear photonic crystal (NPC) slabs. The approach allows one to infiltrate uniformly polystyrene materials that possess large Kerr nonlinearity and ultrafast nonlinear response into the cylindrical air holes with diameter of hundred nanometers that are perforated in silicon membranes. Both the structural characterization via the cross-sectional scanning electron microscopy images and the optical characterization via the transmission spectrum measurement undoubtedly show that the fabricated compound NPC samples have uniform and dense polymer infiltration and are of high quality in optical properties. The compound NPC samples exhibit sharp transmission band edges and nondegraded high quality factor of microcavities compared with those in the bare silicon PC. The versatile method can be expanded to make general semiconductor-polymer hybrid optical nanostructures, and thus it may pave the way for reliable and efficient fabrication of ultrafast and ultralow power all-optical tunable integrated photonic devices and circuits.

Coupling of a high-energy excitation to superconducting quasiparticles in a cuprate from coherent charge fluctuation spectroscopy

PubMed Central

Mansart, Barbara; Lorenzana, José; Mann, Andreas; Odeh, Ahmad; Scarongella, Mariateresa; Chergui, Majed; Carbone, Fabrizio

2013-01-01

Dynamical information on spin degrees of freedom of proteins or solids can be obtained by NMR and electron spin resonance. A technique with similar versatility for charge degrees of freedom and their ultrafast correlations could move the understanding of systems like unconventional superconductors forward. By perturbing the superconducting state in a high-Tc cuprate, using a femtosecond laser pulse, we generate coherent oscillations of the Cooper pair condensate that can be described by an NMR/electron spin resonance formalism. The oscillations are detected by transient broad-band reflectivity and are found to resonate at the typical scale of Mott physics (2.6 eV), suggesting the existence of a nonretarded contribution to the pairing interaction, as in unconventional (non-Migdal–Eliashberg) theories.

Photoinduced Processes in Cobalt-Complexes: Condensed Phase and Gas Phase

NASA Astrophysics Data System (ADS)

Rupp, F.; Chevalier, K.; Wolf, M. M. N.; Krüger, H.-J.; Wüllen, C. v.; Nosenko, Y.; Niedner-Schatteburg, Y.; Riehn, C.; Diller, R.

2013-03-01

Femtosecond time-resolved, steady-state spectroscopic methods and quantum chemical calculations are employed to study ultrafast photoinduced processes in [Co(III)-(L-N4Me2)(dbc)](BPh4) and [Co(II)-(L-N4tBu2)(dbsq)](B(p-C6H4Cl)4) and to characterise the transient redox- and spin-states in condensed and gas phase.

Quantum Zeno Blockade for Next Generation Optical Switching in Fiber Systems

DTIC Science & Technology

2013-09-01

and utilized a self - referential quantum process tomography method to observe the Zeno effect in optical fiber using the ultrafast all- optical switch...controllable and can be used as a knob to study the core physics behind the Zeno-based switching. For this experiment, we developed a self - referential ...efficient optical communications. The quantum Zeno effect can be used to induce or inhibit optical switching through a variety of processes , all of

Electric transport of a single-crystal iron chalcogenide FeSe superconductor: Evidence of symmetry-breakdown nematicity and additional ultrafast Dirac cone-like carriers

NASA Astrophysics Data System (ADS)

Huynh, K. K.; Tanabe, Y.; Urata, T.; Oguro, H.; Heguri, S.; Watanabe, K.; Tanigaki, K.

2014-10-01

An SDW antiferromagnetic (SDW-AF) low-temperature phase transition is generally observed and the AF spin fluctuations are considered to play an important role for the superconductivity pairing mechanism in FeAs superconductors. However, a similar magnetic phase transition is not observed in FeSe superconductors, which has caused considerable discussion. We report on the intrinsic electronic states of FeSe as elucidated by electric transport measurements under magnetic fields using a high quality single crystal. A mobility spectrum analysis, an ab initio method that does not make assumptions on the transport parameters in a multicarrier system, provides very important and clear evidence that another hidden order, most likely the symmetry broken from the tetragonal C4 symmetry to the C2 symmetry nematicity associated with the selective d -orbital splitting, exists in the case of superconducting FeSe other than the AF magnetic order spin fluctuations. The intrinsic low-temperature phase in FeSe is in the almost compensated semimetallic states but is additionally accompanied by Dirac cone-like ultrafast electrons ˜104cm2(VS) -1 as minority carriers.

Photonic crystal fiber technology for compact fiber-delivered high-power ultrafast fiber lasers

NASA Astrophysics Data System (ADS)

Triches, Marco; Michieletto, Mattia; Johansen, Mette M.; Jakobsen, Christian; Olesen, Anders S.; Papior, Sidsel R.; Kristensen, Torben; Bondue, Magalie; Weirich, Johannes; Alkeskjold, Thomas T.

2018-02-01

Photonic crystal fiber (PCF) technology has radically impacted the scientific and industrial ultrafast laser market. Reducing platform dimensions are important to decrease cost and footprint while maintaining high optical efficiency. We present our recent work on short 85 μm core ROD-type fiber amplifiers that maintain single-mode performance and excellent beam quality. Robust long-term performance at 100 W average power and 250 kW peak power in 20 ps pulses at 1030 nm wavelength is presented, exceeding 500 h with stable performance in terms of both polarization and power. In addition, we present our recent results on hollow-core ultrafast fiber delivery maintaining high beam quality and polarization purity.

Sensing Atomic Motion from the Zero Point to Room Temperature with Ultrafast Atom Interferometry.

PubMed

Johnson, K G; Neyenhuis, B; Mizrahi, J; Wong-Campos, J D; Monroe, C

2015-11-20

We sense the motion of a trapped atomic ion using a sequence of state-dependent ultrafast momentum kicks. We use this atom interferometer to characterize a nearly pure quantum state with n=1 phonon and accurately measure thermal states ranging from near the zero-point energy to n[over ¯]~10^{4}, with the possibility of extending at least 100 times higher in energy. The complete energy range of this method spans from the ground state to far outside of the Lamb-Dicke regime, where atomic motion is greater than the optical wavelength. Apart from thermometry, these interferometric techniques are useful for characterizing ultrafast entangling gates between multiple trapped ions.

Asymmetric-detection time-stretch optical microscopy (ATOM) for ultrafast high-contrast cellular imaging in flow

PubMed Central

Wong, Terence T. W.; Lau, Andy K. S.; Ho, Kenneth K. Y.; Tang, Matthew Y. H.; Robles, Joseph D. F.; Wei, Xiaoming; Chan, Antony C. S.; Tang, Anson H. L.; Lam, Edmund Y.; Wong, Kenneth K. Y.; Chan, Godfrey C. F.; Shum, Ho Cheung; Tsia, Kevin K.

2014-01-01

Accelerating imaging speed in optical microscopy is often realized at the expense of image contrast, image resolution, and detection sensitivity – a common predicament for advancing high-speed and high-throughput cellular imaging. We here demonstrate a new imaging approach, called asymmetric-detection time-stretch optical microscopy (ATOM), which can deliver ultrafast label-free high-contrast flow imaging with well delineated cellular morphological resolution and in-line optical image amplification to overcome the compromised imaging sensitivity at high speed. We show that ATOM can separately reveal the enhanced phase-gradient and absorption contrast in microfluidic live-cell imaging at a flow speed as high as ~10 m/s, corresponding to an imaging throughput of ~100,000 cells/sec. ATOM could thus be the enabling platform to meet the pressing need for intercalating optical microscopy in cellular assay, e.g. imaging flow cytometry – permitting high-throughput access to the morphological information of the individual cells simultaneously with a multitude of parameters obtained in the standard assay. PMID:24413677

Theory of low-power ultra-broadband terahertz sideband generation in bi-layer graphene

PubMed Central

Crosse, J. A.; Xu, Xiaodong; Sherwin, Mark S.; Liu, R. B.

2014-01-01

In a semiconductor illuminated by a strong terahertz (THz) field, optically excited electron–hole pairs can recombine to emit light in a broad frequency comb evenly spaced by twice the THz frequency. Such high-order THz sideband generation is of interest both as an example of extreme nonlinear optics and also as a method for ultrafast electro-optical modulation. So far, this phenomenon has only been observed with large field strengths (~10 kV cm−1), an obstacle for technological applications. Here we predict that bi-layer graphene generates high-order sidebands at much weaker THz fields. We find that a THz field of strength 1 kV cm−1 can produce a high-sideband spectrum of about 30 THz, 100 times broader than in GaAs. The sidebands are generated despite the absence of classical collisions, with the quantum coherence of the electron–hole pairs enabling recombination. These remarkable features lower the barrier to desktop electro-optical modulation at THz frequencies, facilitating ultrafast optical communications. PMID:25249245

Ultra-fast three terminal perpendicular spin-orbit torque MRAM (Presentation Recording)

NASA Astrophysics Data System (ADS)

Boulle, Olivier; Cubukcu, Murat; Hamelin, Claire; Lamard, Nathalie; Buda-Prejbeanu, Liliana; Mikuszeit, Nikolai; Garello, Kevin; Gambardella, Pietro; Langer, Juergen; Ocker, Berthold; Miron, Mihai; Gaudin, Gilles

2015-09-01

The discovery that a current flowing in a heavy metal can exert a torque on a neighboring ferromagnet has opened a new way to manipulate the magnetization at the nanoscale. This "spin orbit torque" (SOT) has been demonstrated in ultrathin magnetic multilayers with structural inversion asymmetry (SIA) and high spin orbit coupling, such as Pt/Co/AlOx multilayers. We have shown that this torque can lead to the magnetization switching of a perpendicularly magnetized nanomagnet by an in-plane current injection. The manipulation of magnetization by SOT has led to a novel concept of magnetic RAM memory, the SOT-MRAM, which combines non volatility, high speed, reliability and large endurance. These features make the SOT-MRAM a good candidate to replace SRAM for non-volatile cache memory application. We will present the proof of concept of a perpendicular SOT-MRAM cell composed of a Ta/FeCoB/MgO/FeCoB magnetic tunnel junction and demonstrate ultra-fast (down to 300 ps) deterministic bipolar magnetization switching. Macrospin and micromagnetic simulations including SOT cannot reproduce the experimental results, which suggests that additional physical mechanisms are at stacks. Our results show that SOT-MRAM is fast, reliable and low power, which is promising for non-volatile cache memory application. We will also discuss recent experiments of magnetization reversal in ultrathin multilayers Pt/Co/AlOx by very short (<200 ps) current pulses. We will show that in this material, the Dzyaloshinskii-Moryia interaction plays a key role in the reversal process.

Femtosecond activation of magnetoelectricity

NASA Astrophysics Data System (ADS)

Bossini, D.; Konishi, K.; Toyoda, S.; Arima, T.; Yumoto, J.; Kuwata-Gonokami, M.

2018-04-01

In magnetoelectric and multiferroic materials, the magnetic degree of freedom can be controlled by electric field, and vice versa. A significant amount of research has been devoted to exploiting this effect for magnetoelectric data storage and manipulation devices driven by d.c. electric fields1-4. Aiming at ever-faster schemes of magnetoelectric manipulation, a promising alternative approach offers similar control on a femtosecond timescale, relying on laser pulses4-6 to control both the charge7,8 and the magnetic9,10 order of solids. Here we photo-induce magnetoelectricity and multiferroicity in CuB2O4 on a sub-picosecond timescale. This process is triggered by the resonant optical generation of the highest-energy magnetic excitations—magnons with wavevectors near the edges of the Brillouin zone. The most striking consequence of the photo-excitation is that the absorption of light becomes non-reciprocal, which means that the material exhibits a different transparency for two opposite directions of propagation of light. The photo-induced magnetoelectricity does not show any decay on the picosecond timescale. Our findings uncover a path for ultrafast manipulations of the intrinsic coupling between charges and spins in multiferroics4, which may reveal unexplored magnetic configurations and unravel new functionalities in terms of femtosecond optical control of magnetism.

Lightwave-driven quasiparticle collisions on a sub-cycle timescale

PubMed Central

Langer, F.; Hohenleutner, M.; Schmid, C.; Poellmann, C.; Nagler, P.; Korn, T.; Schüller, C.; Sherwin, M. S.; Huttner, U.; Steiner, J. T.; Koch, S. W.; Kira, M.; Huber, R.

2016-01-01

Ever since Ernest Rutherford first scattered α-particles from gold foils1, collision experiments have revealed unique insights into atoms, nuclei, and elementary particles2. In solids, many-body correlations also lead to characteristic resonances3, called quasiparticles, such as excitons, dropletons4, polarons, or Cooper pairs. Their structure and dynamics define spectacular macroscopic phenomena, ranging from Mott insulating states via spontaneous spin and charge order to high-temperature superconductivity5. Fundamental research would immensely benefit from quasiparticle colliders, but the notoriously short lifetimes of quasiparticles6 have challenged practical solutions. Here we exploit lightwave-driven charge transport7–24, the backbone of attosecond science9–13, to explore ultrafast quasiparticle collisions directly in the time domain: A femtosecond optical pulse creates excitonic electron–hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying wave packet dynamics, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands17–19 of the optical excitation. A full quantum theory explains our observations microscopically. This approach opens the door to collision experiments with a broad variety of complex quasiparticles and suggests a promising new way of sub-femtosecond pulse generation. PMID:27172045

Antiferromagnetic spintronics

NASA Astrophysics Data System (ADS)

Baltz, V.; Manchon, A.; Tsoi, M.; Moriyama, T.; Ono, T.; Tserkovnyak, Y.

2018-01-01

Antiferromagnetic materials could represent the future of spintronic applications thanks to the numerous interesting features they combine: they are robust against perturbation due to magnetic fields, produce no stray fields, display ultrafast dynamics, and are capable of generating large magnetotransport effects. Intense research efforts over the past decade have been invested in unraveling spin transport properties in antiferromagnetic materials. Whether spin transport can be used to drive the antiferromagnetic order and how subsequent variations can be detected are some of the thrilling challenges currently being addressed. Antiferromagnetic spintronics started out with studies on spin transfer and has undergone a definite revival in the last few years with the publication of pioneering articles on the use of spin-orbit interactions in antiferromagnets. This paradigm shift offers possibilities for radically new concepts for spin manipulation in electronics. Central to these endeavors are the need for predictive models, relevant disruptive materials, and new experimental designs. This paper reviews the most prominent spintronic effects described based on theoretical and experimental analysis of antiferromagnetic materials. It also details some of the remaining bottlenecks and suggests possible avenues for future research. This review covers both spin-transfer-related effects, such as spin-transfer torque, spin penetration length, domain-wall motion, and "magnetization" dynamics, and spin-orbit related phenomena, such as (tunnel) anisotropic magnetoresistance, spin Hall, and inverse spin galvanic effects. Effects related to spin caloritronics, such as the spin Seebeck effect, are linked to the transport of magnons in antiferromagnets. The propagation of spin waves and spin superfluids in antiferromagnets is also covered.

Strategies to improve phase-stability of ultrafast swept source optical coherence tomography for single shot imaging of transient mechanical waves at 16 kHz frame rate

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, Shaozhen; Wei, Wei; Hsieh, Bao-Yu

We present single-shot phase-sensitive imaging of propagating mechanical waves within tissue, enabled by an ultrafast optical coherence tomography (OCT) system powered by a 1.628 MHz Fourier domain mode-locked (FDML) swept laser source. We propose a practical strategy for phase-sensitive measurement by comparing the phases between adjacent OCT B-scans, where the B-scan contains a number of A-scans equaling an integer number of FDML buffers. With this approach, we show that micro-strain fields can be mapped with ∼3.0 nm sensitivity at ∼16 000 fps. The system's capabilities are demonstrated on porcine cornea by imaging mechanical wave propagation launched by a pulsed UV laser beam, promisingmore » non-contact, real-time, and high-resolution optical coherence elastography.« less

Tuning the nonlinear response of (6,5)-enriched single-wall carbon nanotubes dispersions

NASA Astrophysics Data System (ADS)

Aréstegui, O. S.; Silva, E. C. O.; Baggio, A. L.; Gontijo, R. N.; Hickmann, J. M.; Fantini, C.; Alencar, M. A. R. C.; Fonseca, E. J. S.

2017-04-01

Ultrafast nonlinear optical properties of (6,5)-enriched single-wall carbon nanotubes (SWCNTs) dispersions are investigated using the thermally managed Z-scan technique. As the (6,5) SWCNTs presented a strong resonance in the range of 895-1048 nm, the nonlinear refractive index (n2) and the absorption coefficients (β) measurements were performed tuning the laser exactly around absorption peak of the (6,5) SWCNTs. It is observed that the nonlinear response is very sensitive to the wavelength and the spectral behavior of n2 is strongly correlated to the tubes one-photon absorption band, presenting also a peak when the laser photon energy is near the tube resonance energy. This result suggests that a suitable selection of nanotubes types may provide optimized nonlinear optical responses in distinct regions of the electromagnetic spectrum. Analysis of the figures of merit indicated that this material is promising for ultrafast nonlinear optical applications under near infrared excitation.

Optical imaging through turbid media with a degenerate four-wave mixing correlation time gate

DOEpatents

Sappey, Andrew D.

1998-04-14

Optical imaging through turbid media is demonstrated using a degenerate four-wave mixing correlation time gate. An apparatus and method for detecting ballistic and/or snake light while rejecting unwanted diffusive light for imaging structures within highly scattering media are described. Degenerate four-wave mixing (DFWM) of a doubled YAG laser in rhodamine 590 is used to provide an ultrafast correlation time gate to discriminate against light that has undergone multiple scattering and therefore has lost memory of the structures within the scattering medium. Images have been obtained of a test cross-hair pattern through highly turbid suspensions of whole milk in water that are opaque to the naked eye, which demonstrates the utility of DFWM for imaging through turbid media. Use of DFWM as an ultrafast time gate for the detection of ballistic and/or snake light in optical mammography is discussed.

Circularly polarized attosecond pulse generation and applications to ultrafast magnetism

NASA Astrophysics Data System (ADS)

Bandrauk, André D.; Guo, Jing; Yuan, Kai-Jun

2017-12-01

Attosecond science is a growing new field of research and potential applications which relies on the development of attosecond light sources. Achievements in the generation and application of attosecond pulses enable to investigate electron dynamics in the nonlinear nonperturbative regime of laser-matter interactions on the electron’s natural time scale, the attosecond. In this review, we describe the generation of circularly polarized attosecond pulses and their applications to induce attosecond magnetic fields, new tools for ultrafast magnetism. Simulations are performed on aligned one-electron molecular ions by using nonperturbative nonlinear solutions of the time-dependent Schrödinger equation. We discuss how bichromatic circularly polarized laser pulses with co-rotating or counter-rotating components induce electron-parent ion recollisions, thus producing circularly polarized high-order harmonic generation, the source of circularly polarized attosecond pulses. Ultrafast quantum electron currents created by the generated attosecond pulses give rise to attosecond magnetic field pulses. The results provide a guiding principle for producing circularly polarized attosecond pulses and ultrafast magnetic fields in complex molecular systems for future research in ultrafast magneto-optics.

Subpicosecond Optical Digital Computation Using Conjugate Parametric Generators

DTIC Science & Technology

1989-03-31

Using Phase Conjugate Farametric Generators ..... 12. PERSONAL AUTHOR(S) Alfano, Robert- Eichmann . George; Dorsinville. Roger! Li. Yao 13a. TYPE OF...conjugation-based optical residue arithmetic processor," Y. Li, G. Eichmann , R. Dorsinville, and R. R. Alfano, Opt. Lett. 13, (1988). [2] "Parallel ultrafast...optical digital and symbolic computation via optical phase conjugation," Y. Li, G. Eichmann , R. Dorsinville, Appl. Opt. 27, 2025 (1988). [3

Brightened spin-triplet interlayer excitons and optical selection rules in van der Waals heterobilayers

NASA Astrophysics Data System (ADS)

Yu, Hongyi; Liu, Gui-Bin; Yao, Wang

2018-07-01

We investigate the optical properties of spin-triplet interlayer excitons in heterobilayer transition metal dichalcogenides in comparison with the spin-singlet ones. Surprisingly, the optical transition dipole of the spin-triplet exciton is found to be in the same order of magnitude to that of the spin-singlet exciton, in sharp contrast to the monolayer excitons where the spin-triplet species is considered as dark compared to the singlet. Unlike the monolayer excitons whose spin-conserved (spin-flip) transition dipole can only couple to light of in-plane (out-of-plane) polarisation, such restriction is removed for the interlayer excitons due to the breaking of the out-of-plane mirror symmetry. We find that as the interlayer atomic registry changes, the optical transition dipole of interlayer exciton crosses between in-plane ones of opposite circular polarizations and the out-of-plane one for both the spin-triplet and spin-singlet species. As a result, excitons of both species have non-negligible coupling into photon modes of both in-plane and out-of-plane propagations, another sharp difference from the monolayers where the exciton couples predominantly into the out-of-plane propagation channel. At given atomic registry, the spin-triplet and spin-singlet excitons have distinct valley polarisation selection rules, allowing the selective optical addressing of both the valley configuration and the spin-singlet/triplet configuration of interlayer excitons.

Nuclear Spin Nanomagnet in an Optically Excited Quantum Dot

NASA Astrophysics Data System (ADS)

Korenev, V. L.

2007-12-01

Linearly polarized light tuned slightly below the optical transition of the negatively charged exciton (trion) in a single quantum dot causes the spontaneous nuclear spin polarization (self-polarization) at a level close to 100%. The effective magnetic field of spin-polarized nuclei shifts the optical transition energy close to resonance with photon energy. The resonantly enhanced Overhauser effect sustains the stability of the nuclear self-polarization even in the absence of spin polarization of the quantum dot electron. As a result the optically selected single quantum dot represents a tiny magnet with the ferromagnetic ordering of nuclear spins—the nuclear spin nanomagnet.

Selective Optical Addressing of Nuclear Spins through Superhyperfine Interaction in Rare-Earth Doped Solids.

PubMed

Car, B; Veissier, L; Louchet-Chauvet, A; Le Gouët, J-L; Chanelière, T

2018-05-11

In Er^{3+}:Y_{2}SiO_{5}, we demonstrate the selective optical addressing of the ^{89}Y^{3+} nuclear spins through their superhyperfine coupling with the Er^{3+} electronic spins possessing large Landé g factors. We experimentally probe the electron-nuclear spin mixing with photon echo techniques and validate our model. The site-selective optical addressing of the Y^{3+} nuclear spins is designed by adjusting the magnetic field strength and orientation. This constitutes an important step towards the realization of long-lived solid-state qubits optically addressed by telecom photons.

Selective Optical Addressing of Nuclear Spins through Superhyperfine Interaction in Rare-Earth Doped Solids

NASA Astrophysics Data System (ADS)

Car, B.; Veissier, L.; Louchet-Chauvet, A.; Le Gouët, J.-L.; Chanelière, T.

2018-05-01

In Er3 +:Y2SiO5 , we demonstrate the selective optical addressing of the Y89 3 + nuclear spins through their superhyperfine coupling with the Er3 + electronic spins possessing large Landé g factors. We experimentally probe the electron-nuclear spin mixing with photon echo techniques and validate our model. The site-selective optical addressing of the Y3 + nuclear spins is designed by adjusting the magnetic field strength and orientation. This constitutes an important step towards the realization of long-lived solid-state qubits optically addressed by telecom photons.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kfir, Ofer, E-mail: ofertx@technion.ac.il, E-mail: oren@si.technion.ac.il; Bordo, Eliyahu; Ilan Haham, Gil

The recent demonstration of bright circularly polarized high-order harmonics of a bi-circular pump field gave rise to new opportunities in ultrafast chiral science. In previous works, the required nontrivial bi-circular pump field was produced using a relatively complicated and sensitive Mach-Zehnder-like interferometer. We propose a compact and stable in-line apparatus for converting a quasi-monochromatic linearly polarized ultrashort driving laser field into a bi-circular field and employ it for generation of helically polarized high-harmonics. Furthermore, utilizing the apparatus for a spectroscopic spin-mixing measurement, we identify the photon spins of the bi-circular weak component field that are annihilated during the high harmonicsmore » process.« less

Tunable and switchable dual-waveband ultrafast fiber laser with 100 GHz repetition-rate.

PubMed

Tan, Xiao-Mei; Chen, Hong-Jie; Cui, Hu; Lv, Yao-Kun; Zhao, Guan-Kai; Luo, Zhi-Chao; Luo, Ai-Ping; Xu, Wen-Cheng

2017-07-10

We demonstrate a tunable and switchable dual-waveband 100 GHz high-repetition-rate (HRR) ultrafast fiber laser based on dissipative four-wave-mixing (DFWM) mode-locked technique. Each waveband maintains HRR operation. The DFWM effect was realized by combining a Fabry-Perot (F-P) filter and a piece of highly nonlinear fiber (HNLF). The tunable and switchable operations were achieved by nonlinear polarization rotation (NPR) technique. Through appropriately controlling the filtering effect induced by NPR, the laser could operate at two kinds of tunable regimes. One is that the spacing between these two wavebands could be tuned while keeping their center at 1559 nm. The other is that the central position of the entire dual-waveband is tunable while with the same separation between these two wavebands of 13.2 nm. Moreover, the laser could switch between these two wavebands. Correspondingly, the center of the single-waveband has a tuning range of 15.2 nm. This versatile ultrafast fiber laser may find applications in fields of optical frequency combs, high speed optical communications, where HRR pulses are necessary.

Ultrafast Spectroscopic Noninvasive Probe of Vertical Carrier Transport in Heterostructure Devices (Second year of three year progress report)

DTIC Science & Technology

2014-10-01

properties in Army-relevant semiconductor materials and optoelectronic ( OE ) devices by developing and applying ultrafast optical spectroscopy techniques...met our Q6 through Q8 goals of incorporating electrical testing capabilities into our system, investigating OE devices under operating conditions...extending the capabilities of our system into the IR range, and investigating new OE devices. We have made significant progress towards our Q5 goal of

Ultrafast Spectroscopy of Mid-Infrared Semiconductors Using the Signal and Idler Beams of a Synchronous Optical Parametric Oscillator

DTIC Science & Technology

2008-03-01

then used to fit theoretical models describing radiative and non-radiative relaxation processes. 3.2 Experimental Setup This thesis uses a mode...Russian Efforts. Master’s thesis, Naval Postgraduate School, 2005. 5. Chirsto, Farid C. “Thermochemistry and Kinetics Models for MagnesiumTe- flon/Viton...Coherent Mira Model 900-F Laser. 7. Cooley, William T. Measurement of Ultrafast Carrier Recombination Dynamics in Mid-Infrared Semiconductor Laser Material

Bias Dependent Spin Relaxation in a [110]-InAs/AlSb Two Dimensional Electron System

NASA Astrophysics Data System (ADS)

Hicks, J.; Holabird, K.

2005-03-01

Manipulation of electron spin is a critical component of many proposed semiconductor spintronic devices. One promising approach utilizes the Rashba effect by which an applied electric field can be used to reduce the spin lifetime or rotate spin orientation through spin-orbit interaction. The large spin-orbit interaction needed for this technique to be effective typically leads to fast spin relaxation through precessional decay, which may severely limit device architectures and functionalities. An exception arises in [110]-oriented heterostructures where the crystal magnetic field associated with bulk inversion asymmetry lies along the growth direction and in which case spins oriented along the growth direction do not precess. These considerations have led to a recent proposal of a spin-FET that incorporates a [110]-oriented, gate-controlled InAs quantum well channel [1]. We report measurements of the electron spin lifetime as a function of applied electric field in a [110]-InAs 2DES. Measurements made using an ultrafast, mid-IR pump-probe technique indicate that the spin lifetime can be reduced from its maximum to minimum value over a range of less than 0.2V per quantum well at room temperature. This work is supported by DARPA, NSERC and the NSF grant ECS - 0322021. [1] K. C. Hall, W. H. Lau, K. Gundogdu, M. E. Flatte, and T. F. Boggess, Appl. Phys. Lett. 83, 2937 (2003).

Universal Behavior of Quantum Spin Liquid and Optical Conductivity in the Insulator Herbertsmithite

NASA Astrophysics Data System (ADS)

Shaginyan, V. R.; Msezane, A. Z.; Stephanovich, V. A.; Popov, K. G.; Japaridze, G. S.

2018-04-01

We analyze optical conductivity with the goal to demonstrate experimental manifestation of a new state of matter, the so-called fermion condensate. Fermion condensates are realized in quantum spin liquids, exhibiting typical behavior of heavy-fermion metals. Measurements of the low-frequency optical conductivity collected on the geometrically frustrated insulator herbertsmithite provide important experimental evidence of the nature of its quantum spin liquid composed of spinons. To analyze recent measurements of the herbertsmithite optical conductivity at different temperatures, we employ a model of strongly correlated quantum spin liquid located near the fermion condensation phase transition. Our theoretical analysis of the optical conductivity allows us to expose the physical mechanism of its temperature dependence. We also predict a dependence of the optical conductivity on a magnetic field. We consider an experimental manifestation (optical conductivity) of a new state of matter (so-called fermion condensate) realized in quantum spin liquids, for, in many ways, they exhibit typical behavior of heavy-fermion metals. Measurements of the low-frequency optical conductivity collected on the geometrically frustrated insulator herbertsmithite produce important experimental evidence of the nature of its quantum spin liquid composed of spinons. To analyze recent measurements of the herbertsmithite optical conductivity at different temperatures, we employ a model of a strongly correlated quantum spin liquid located near the fermion condensation phase transition. Our theoretical analysis of the optical conductivity allows us to reveal the physical mechanism of its temperature dependence. We also predict a dependence of the optical conductivity on a magnetic field.

Non-binary Colour Modulation for Display Device Based on Phase Change Materials.

PubMed

Ji, Hong-Kai; Tong, Hao; Qian, Hang; Hui, Ya-Juan; Liu, Nian; Yan, Peng; Miao, Xiang-Shui

2016-12-19

A reflective-type display device based on phase change materials is attractive because of its ultrafast response time and high resolution compared with a conventional display device. This paper proposes and demonstrates a unique display device in which multicolour changing can be achieved on a single device by the selective crystallization of double layer phase change materials. The optical contrast is optimized by the availability of a variety of film thicknesses of two phase change layers. The device exhibits a low sensitivity to the angle of incidence, which is important for display and colour consistency. The non-binary colour rendering on a single device is demonstrated for the first time using optical excitation. The device shows the potential for ultrafast display applications.

Modified two-photon absorption and dispersion of ultrafast third-order polarization beats via twin noisy driving fields

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang Yanpeng; Department of Electronic Science and Technology, Xi'an Jiaotong University, Xi'an 710049; Gan Chenli

2006-05-15

We investigate the color-locked twin-noisy-field correlation effects in third-order nonlinear absorption and dispersion of ultrafast polarization beats. We demonstrate a phase-sensitive method for studying the two-photon nondegenerate four-wave mixing (NDFWM) due to atomic coherence in a multilevel system. The reference signal is another one-photon degenerate four-wave-mixing signal, which propagates along the same optical path as the NDFWM signal. This method is used for studying the phase dispersion of the third-order susceptibility and for the optical heterodyne detection of the NDFWM signal. The third-order nonlinear response can be controlled and modified through the color-locked correlation of twin noisy fields.

Drude weight and optical conductivity of a two-dimensional heavy-hole gas with k-cubic spin-orbit interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mawrie, Alestin; Ghosh, Tarun Kanti

We present a detailed theoretical study on zero-frequency Drude weight and optical conductivity of a two-dimensional heavy-hole gas (2DHG) with k-cubic Rashba and Dresselhaus spin-orbit interactions. The presence of k-cubic spin-orbit couplings strongly modifies the Drude weight in comparison to the electron gas with k-linear spin-orbit couplings. For large hole density and strong k-cubic spin-orbit couplings, the density dependence of Drude weight deviates from the linear behavior. We establish a relation between optical conductivity and the Berry connection. Unlike two-dimensional electron gas with k-linear spin-orbit couplings, we explicitly show that the optical conductivity does not vanish even for equal strengthmore » of the two spin-orbit couplings. We attribute this fact to the non-zero Berry phase for equal strength of k-cubic spin-orbit couplings. The least photon energy needed to set in the optical transition in hole gas is one order of magnitude smaller than that of electron gas. Types of two van Hove singularities appear in the optical spectrum are also discussed.« less

Ultrafast creation of large Schrödinger cat states of an atom.

PubMed

Johnson, K G; Wong-Campos, J D; Neyenhuis, B; Mizrahi, J; Monroe, C

2017-09-26

Mesoscopic quantum superpositions, or Schrödinger cat states, are widely studied for fundamental investigations of quantum measurement and decoherence as well as applications in sensing and quantum information science. The generation and maintenance of such states relies upon a balance between efficient external coherent control of the system and sufficient isolation from the environment. Here we create a variety of cat states of a single trapped atom's motion in a harmonic oscillator using ultrafast laser pulses. These pulses produce high fidelity impulsive forces that separate the atom into widely separated positions, without restrictions that typically limit the speed of the interaction or the size and complexity of the resulting motional superposition. This allows us to quickly generate and measure cat states larger than previously achieved in a harmonic oscillator, and create complex multi-component superposition states in atoms.Generation of mesoscopic quantum superpositions requires both reliable coherent control and isolation from the environment. Here, the authors succeed in creating a variety of cat states of a single trapped atom, mapping spin superpositions into spatial superpositions using ultrafast laser pulses.

Electron spin dynamics and optical orientation of Mn2+ ions in GaAs

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; Yakovlev, D. R.; Bayer, M.

2013-04-01

We present an overview of spin-related phenomena in GaAs doped with low concentration of Mn-acceptors (below 1018 cm-3). We use the combination of different experimental techniques such as spin-flip Raman scattering and time-resolved photoluminescence. This allows to evaluate the time evolution of both electron and Mn spins. We show that optical orientation of Mn ions is possible under application of weak magnetic field, which is required to suppress the manganese spin relaxation. The optically oriented Mn2+ ions maintain the spin and return part of the polarization back to the electron spin system providing a long-lived electron spin memory. This leads to a bunch of spectacular effects such as non-exponential electron spin decay and spin precession in the effective exchange fields.

A Solution-Processed Ultrafast Optical Switch Based on a Nanostructured Epsilon-Near-Zero Medium.

PubMed

Guo, Qiangbing; Cui, Yudong; Yao, Yunhua; Ye, Yuting; Yang, Yue; Liu, Xueming; Zhang, Shian; Liu, Xiaofeng; Qiu, Jianrong; Hosono, Hideo

2017-07-01

All the optical properties of materials are derived from dielectric function. In spectral region where the dielectric permittivity approaches zero, known as epsilon-near-zero (ENZ) region, the propagating light within the material attains a very high phase velocity, and meanwhile the material exhibits strong optical nonlinearity. The interplay between the linear and nonlinear optical response in these materials thus offers unprecedented pathways for all-optical control and device design. Here the authors demonstrate ultrafast all-optical modulation based on a typical ENZ material of indium tin oxide (ITO) nanocrystals (NCs), accessed by a wet-chemistry route. In the ENZ region, the authors find that the optical response in these ITO NCs is associated with a strong nonlinear character, exhibiting sub-picosecond response time (corresponding to frequencies over 2 THz) and modulation depth up to ≈160%. This large optical nonlinearity benefits from the highly confined geometry in addition to the ENZ enhancement effect of the ITO NCs. Based on these ENZ NCs, the authors successfully demonstrate a fiber optical switch that allows switching of continuous laser wave into femtosecond laser pulses. Combined with facile processibility and tunable optical properties, these solution-processed ENZ NCs may offer a scalable and printable material solution for dynamic photonic and optoelectronic devices. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Coherent Spin Control at the Quantum Level in an Ensemble-Based Optical Memory.

PubMed

Jobez, Pierre; Laplane, Cyril; Timoney, Nuala; Gisin, Nicolas; Ferrier, Alban; Goldner, Philippe; Afzelius, Mikael

2015-06-12

Long-lived quantum memories are essential components of a long-standing goal of remote distribution of entanglement in quantum networks. These can be realized by storing the quantum states of light as single-spin excitations in atomic ensembles. However, spin states are often subjected to different dephasing processes that limit the storage time, which in principle could be overcome using spin-echo techniques. Theoretical studies suggest this to be challenging due to unavoidable spontaneous emission noise in ensemble-based quantum memories. Here, we demonstrate spin-echo manipulation of a mean spin excitation of 1 in a large solid-state ensemble, generated through storage of a weak optical pulse. After a storage time of about 1 ms we optically read-out the spin excitation with a high signal-to-noise ratio. Our results pave the way for long-duration optical quantum storage using spin-echo techniques for any ensemble-based memory.

Magneto-optical studies of quantum dots

NASA Astrophysics Data System (ADS)

Russ, Andreas Hans

Significant effort in condensed matter physics has recently been devoted to the field of "spintronics" which seeks to utilize the spin degree of freedom of electrons. Unlike conventional electronics that rely on the electron charge, devices exploiting their spin have the potential to yield new and novel technological applications, including spin transistors, spin filters, and spin-based memory devices. Any such application has the following essential requirements: 1) Efficient electrical injection of spin-polarized carriers; 2) Long spin lifetimes; 3) Ability to control and manipulate electron spins; 4) Effective detection of spin-polarized carriers. Recent work has demonstrated efficient electrical injection from ferromagnetic contacts such as Fe and MnAs, utilizing a spin-Light Emitting Diode (spin-LED) as a method of detection. Semiconductor quantum dots (QDs) are attractive candidates for satisfying requirements 2 and 3 as their zero dimensionality significantly suppresses many spin-flip mechanisms leading to long spin coherence times, as well as enabling the localization and manipulation of a controlled number of electrons and holes. This thesis is composed of three projects that are all based on the optical properties of QD structures including: I) Intershell exchange between spin-polarized electrons occupying adjacent shells in InAs QDs; II) Spin-polarized multiexitons in InAs QDs in the presence of spin-orbit interactions; III) The optical Aharonov-Bohm effect in AlxGa1-xAs/AlyGa1-yAs quantum wells (QWs). In the following we introduce some of the basic optical properties of quantum dots, describe the main tool (spin-LED) employed in this thesis to inject and detect spins in these QDs, and conclude with the optical Aharonov-Bohm effect (OAB) in type-II QDs.

Resonant optical spectroscopy and coherent control of C r4 + spin ensembles in SiC and GaN

NASA Astrophysics Data System (ADS)

Koehl, William F.; Diler, Berk; Whiteley, Samuel J.; Bourassa, Alexandre; Son, N. T.; Janzén, Erik; Awschalom, David D.

2017-01-01

Spins bound to point defects are increasingly viewed as an important resource for solid-state implementations of quantum information and spintronic technologies. In particular, there is a growing interest in the identification of new classes of defect spin that can be controlled optically. Here, we demonstrate ensemble optical spin polarization and optically detected magnetic resonance (ODMR) of the S = 1 electronic ground state of chromium (C r4 + ) impurities in silicon carbide (SiC) and gallium nitride (GaN). Spin polarization is made possible by the narrow optical linewidths of these ensembles (<8.5 GHz), which are similar in magnitude to the ground state zero-field spin splitting energies of the ions at liquid helium temperatures. This allows us to optically resolve individual spin sublevels within the ensembles at low magnetic fields using resonant excitation from a cavity-stabilized, narrow-linewidth laser. Additionally, these near-infrared emitters possess exceptionally weak phonon sidebands, ensuring that >73% of the overall optical emission is contained with the defects' zero-phonon lines. These characteristics make this semiconductor-based, transition metal impurity system a promising target for further study in the ongoing effort to integrate optically active quantum states within common optoelectronic materials.

Suppression of spin and optical gaps in phosphorene quantum dots

NASA Astrophysics Data System (ADS)

Zhang, Yingjie; Sheng, Weidong

2018-05-01

Electronic structure and optical properties of triangular phosphorene quantum dots have been investigated theoretically. Based on systematic configuration interaction calculations, the ground and excited states of the interacting many-electron system together with its optical absorption spectrum are obtained. For the nanodot with 60 phosphorus atoms in various dielectric environments, it is found that the spin gap of the correlated system surprisingly overlaps its optical gap over a large range of the effective dielectric constant. The overlapping of the spin and optical gaps can be attributed to the fact that the extra correlation energy in the spin singlet almost compensates the exchange energy in the spin triplet in the presence of strong long-range electron-electron interactions. Moreover, both the spin and optical gaps are shown to be greatly suppressed as the screening effect becomes strong. When the dielectric constant decreases below 2.65, it is seen that the spin gap becomes negative and the quantum dot undergoes a phase transition from nonmagnetic to ferromagnetic. Our results are compared with the previous experimental and theoretical works.

Evidence of an Improper Displacive Phase Transition in Cd2 Re2 O7 via Time-Resolved Coherent Phonon Spectroscopy

NASA Astrophysics Data System (ADS)

Harter, J. W.; Kennes, D. M.; Chu, H.; de la Torre, A.; Zhao, Z. Y.; Yan, J.-Q.; Mandrus, D. G.; Millis, A. J.; Hsieh, D.

2018-01-01

We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at Tc=200 K in the strongly spin-orbit coupled correlated metal Cd2 Re2 O7 . We establish that the structural distortion at Tc is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near Tc. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters.

Continuous wave protocol for simultaneous polarization and optical detection of P1-center electron spin resonance

NASA Astrophysics Data System (ADS)

Kamp, E. J.; Carvajal, B.; Samarth, N.

2018-01-01

The ready optical detection and manipulation of bright nitrogen vacancy center spins in diamond plays a key role in contemporary quantum information science and quantum metrology. Other optically dark defects such as substitutional nitrogen atoms (`P1 centers') could also become potentially useful in this context if they could be as easily optically detected and manipulated. We develop a relatively straightforward continuous wave protocol that takes advantage of the dipolar coupling between nitrogen vacancy and P1 centers in type 1b diamond to detect and polarize the dark P1 spins. By combining mutual spin flip transitions with radio frequency driving, we demonstrate the simultaneous optical polarization and detection of the electron spin resonance of the P1 center. This technique should be applicable to detecting and manipulating a broad range of dark spin populations that couple to the nitrogen vacancy center via dipolar fields, allowing for quantum metrology using these spin populations.

Aspects of Dzyaloshinskii-Moriya Interaction in Two Dimensional Magnetic Structures

NASA Astrophysics Data System (ADS)

Kundu, Anirban

Research on topologically protected chiral magnetic structures such as magnetic domain walls (DWs) and skyrmions, have gained extensive interest because of their possible applications in magnetic data storage industries. The recently observed chiral DW structures in ultrathin ferromagnetic lms with perpendicular magnetic anisotropy has been attributed to the presence of a strong Dzyaloshinskii-Moriya interaction (DMI). In this thesis, the DMI mediated by the conduction electrons in two dimensional magnetic systems such as magnetic thin lms or at the interfaces between two magnetic materials has been studied. I calculate the Ruderman-Kittel- Kasuya-Yosida (RKKY) type indirect exchange coupling between two magnetic moments at nite temperature using the free electron band. At high temperature, the coupling strength decays with distance faster than the coupling at zero temperature but the period of oscillation remains same. However, the free electron band alone could not produce DMI. In the next step, I show addition of Rashba spin-orbit coupling (RSOC) with the spin-polarized conduction electron band produces the DMI between two magnetic ions. The essential feature of this DMI is: the coupling strength increases with the strength of RSOC, but decreases signi cantly with the Heisenberg exchange coupling. The DMI calculated with this model well explains the possibility of preferred Neel or Bloch DW structures with specifc chirality. In addition: I study switching of magnetization with ultrafast laser pulse by inverse Faraday e ect (IFE) where an optically induced non-equilibrium orbital momentum generates an e ective magnetic eld via spin-orbit coupling for magnetization switching. I calculate the magnitude of induced orbital moment for the generic itinerant band and show that magnitude is not large enough to make the switching by a single pulse, however, switching could be possible if multiple pulses are applied to the material.

Selective excitation enables assignment of proton resonances and {sup 1}H-{sup 1}H distance measurement in ultrafast magic angle spinning solid state NMR spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Rongchun; Ramamoorthy, Ayyalusamy, E-mail: ramamoor@umich.edu

2015-07-21

Remarkable developments in ultrafast magic angle spinning (MAS) solid-state NMR spectroscopy enabled proton-based high-resolution multidimensional experiments on solids. To fully utilize the benefits rendered by proton-based ultrafast MAS experiments, assignment of {sup 1}H resonances becomes absolutely necessary. Herein, we propose an approach to identify different proton peaks by using dipolar-coupled heteronuclei such as {sup 13}C or {sup 15}N. In this method, after the initial preparation of proton magnetization and cross-polarization to {sup 13}C nuclei, transverse magnetization of desired {sup 13}C nuclei is selectively prepared by using DANTE (Delays Alternating with Nutations for Tailored Excitation) sequence and then, it is transferredmore » to bonded protons with a short-contact-time cross polarization. Our experimental results demonstrate that protons bonded to specific {sup 13}C atoms can be identified and overlapping proton peaks can also be assigned. In contrast to the regular 2D HETCOR experiment, only a few 1D experiments are required for the complete assignment of peaks in the proton spectrum. Furthermore, the finite-pulse radio frequency driven recoupling sequence could be incorporated right after the selection of specific proton signals to monitor the intensity buildup for other proton signals. This enables the extraction of {sup 1}H-{sup 1}H distances between different pairs of protons. Therefore, we believe that the proposed method will greatly aid in fast assignment of peaks in proton spectra and will be useful in the development of proton-based multi-dimensional solid-state NMR experiments to study atomic-level resolution structure and dynamics of solids.« less

Effectively Single-Mode Self-Recovering Ultrafast Nonlinear Nanowire Surface Plasmons

NASA Astrophysics Data System (ADS)

Tuniz, Alessandro; Weidlich, Stefan; Schmidt, Markus A.

2018-04-01

We report on a regime for surface-plasmon propagation, which is robust to defects and effectively single mode, and we exploit it for accessing the ultrafast nonlinear response of gold on centimeter-long subwavelength-diameter cylindrical nanowires. The hybrid plasmonic-photonic platform is formed by a gold nanowire, monolithically integrated into the core of an optical fiber. We show that, despite the dual-waveguide nature of this structure, the long-range surface plasmon is the only effectively propagating mode in the near infrared, which self-recovers in the presence of gaps via a light-recapturing effect. This self-recovery overcomes detrimental effects of wire discontinuities and enables measurements of the ultrafast nonlinearity of gold, which we perform for a 28-fs pulse duration.

Ultrafast electron transport across nano gaps in nanowire circuits

DOE Office of Scientific and Technical Information (OSTI.GOV)

Potma, Eric O.

In this Program we aim for a closer look at electron transfer through single molecules. To achieve this, we use ultrafast laser pulses to time stamp an electron tunneling event in a molecule that is connected between two metallic electrodes, while reading out the electron current. A key aspect of this project is the use of metallic substrates with plasmonic activity to efficiently manipulate the tunneling probability. The first Phase of this program is concerned with developing highly sensitive tools for the ultrafast optical manipulation of tethered molecules through the evanescent surface field of plasmonic substrates. The second Phase ofmore » the program aims to use these tools for exercising control over the electron tunneling probability.« less

Ultrafast Terahertz Nonlinear Optics of Landau Level Transitions in a Monolayer Graphene

NASA Astrophysics Data System (ADS)

Yumoto, Go; Matsunaga, Ryusuke; Hibino, Hiroki; Shimano, Ryo

2018-03-01

We investigated the ultrafast terahertz (THz) nonlinearity in a monolayer graphene under the strong magnetic field using THz pump-THz probe spectroscopy. An ultrafast suppression of the Faraday rotation associated with inter-Landau level (LL) transitions is observed, reflecting the Dirac electron character of nonequidistant LLs with large transition dipole moments. A drastic modulation of electron distribution in LLs is induced by far off-resonant THz pulse excitation in the transparent region. Numerical simulation based on the density matrix formalism without rotating-wave approximation reproduces the experimental results. Our results indicate that the strong light-matter coupling regime is realized in graphene, with the Rabi frequency exceeding the carrier wave frequency and even the relevant energy scale of the inter-LL transition.

Optical pumping of electron and nuclear spin in a negatively-charged quantum dot

NASA Astrophysics Data System (ADS)

Bracker, Allan; Gershoni, David; Korenev, Vladimir

2005-03-01

We report optical pumping of electron and nuclear spins in an individual negatively-charged quantum dot. With a bias-controlled heterostructure, we inject one electron into the quantum dot. Intense laser excitation produces negative photoluminescence polarization, which is easily erased by the Hanle effect, demonstrating optical pumping of a long-lived resident electron. The electron spin lifetime is consistent with the influence of nuclear spin fluctuations. Measuring the Overhauser effect in high magnetic fields, we observe a high degree of nuclear spin polarization, which is closely correlated to electron spin pumping.

Spin temperature concept verified by optical magnetometry of nuclear spins

NASA Astrophysics Data System (ADS)

Vladimirova, M.; Cronenberger, S.; Scalbert, D.; Ryzhov, I. I.; Zapasskii, V. S.; Kozlov, G. G.; Lemaître, A.; Kavokin, K. V.

2018-01-01

We develop a method of nonperturbative optical control over adiabatic remagnetization of the nuclear spin system and apply it to verify the spin temperature concept in GaAs microcavities. The nuclear spin system is shown to exactly follow the predictions of the spin temperature theory, despite the quadrupole interaction that was earlier reported to disrupt nuclear spin thermalization. These findings open a way for the deep cooling of nuclear spins in semiconductor structures, with the prospect of realizing nuclear spin-ordered states for high-fidelity spin-photon interfaces.

Ultrafast polarisation spectroscopy of photoinduced charges in a conjugated polymer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bakulin, A A; Loosdrecht, P van; Pshenichnikov, M S

2009-07-31

Tunable optical parametric generators and amplifiers (OPA), proposed and developed by Akhmanov and his colleagues, have become the working horses in exploration of dynamical processes in physics, chemistry, and biology. In this paper, we demonstrate the possibility of using ultrafast polarisation-sensitive two-colour spectroscopy, performed with a set of two OPAs, to study charge photogeneration and transport in conjugated polymers and their donor-acceptor blends. (special issue devoted to the 80th birthday of S.A. Akhmanov)

Engineered Multifunctional Nanophotonic Materials for Ultrafast Optical Switching

DTIC Science & Technology

2012-11-02

and Co3 + placed at tetrahedral and octahedral sites, respectively. Single -layer thin films of Co3O4 nanoparticles have large optical nonlinearity and...the first two methodologies in systems having weakly resonant structures, including 3-D and/or 1-D photonic crystal structures (i.e. nonlinear Bragg...Nonlinear optical transmission of lead phthalocyanine-doped nematic liquid crystal composites for multiscale nonlinear switching from nanosecond to

Ultrafast optical modulation of magneto-optical terahertz effects occurring in a graphene-loaded resonant metasurface

NASA Astrophysics Data System (ADS)

Zanotto, S.; Lange, C.; Maag, T.; Pitanti, A.; Miseikis, V.; Coletti, C.; Degl'Innocenti, R.; Baldacci, L.; Huber, R.; Tredicucci, A.

2016-09-01

In this paper we investigate the effect of a static magnetic field and of optical pumping on the transmittance of a hybrid graphene-split ring resonator metasurface. A significant modulation of the transmitted spectra is obtained, both by optical pumping, and by a combination of optical pumping and magnetostatic biasing. The transmittance modulation features spectral fingerprints that are characteristic of a non-trivial interplay between the bare graphene response and the split ring resonance.

Probing Ultrafast Electron Dynamics at Surfaces Using Soft X-Ray Transient Reflectivity Spectroscopy

NASA Astrophysics Data System (ADS)

Baker, L. Robert; Husek, Jakub; Biswas, Somnath; Cirri, Anthony

The ability to probe electron dynamics with surface sensitivity on the ultrafast time scale is critical for understanding processes such as charge separation, injection, and surface trapping that mediate efficiency in catalytic and energy conversion materials. Toward this goal, we have developed a high harmonic generation (HHG) light source for femtosecond soft x-ray reflectivity. Using this light source we investigated the ultrafast carrier dynamics at the surface of single crystalline α-Fe2O3, polycrystalline α-Fe2O3, and the mixed metal oxide, CuFeO2. We have recently demonstrated that CuFeO2 in particular is a selective catalyst for photo-electrochemical CO2 reduction to acetate; however, the role of electronic structure and charge carrier dynamics in mediating catalytic selectivity has not been well understood. Soft x-ray reflectivity measurements probe the M2,3, edges of the 3d transition metals, which provide oxidation and spin state resolution with element specificity. In addition to chemical state specificity, these measurements are also surface sensitive, and by independently simulating the contributions of the real and imaginary components of the complex refractive index, we can differentiate between surface and sub-surface contributions to the excited state spectrum. Accordingly, this work demonstrates the ability to probe ultrafast carrier dynamics in catalytic materials with element and chemical state specificity and with surface sensitivity.

Ultrafast Generation of Large Schrodinger Cat States

NASA Astrophysics Data System (ADS)

Johnson, Kale; Neyenhuis, Brian; Wong-Campos, David; Mizrahi, Jonathan; Campbell, Wes; Monroe, Christopher

2014-05-01

Using a series of spin-dependent kicks on a trapped Yb + ion, we create large, entangled, Schrodinger cat states. We prepare the ion in a superposition of its two mf = 0 hyperfine ground states, representing an effective spin-1/2 system. Trapped in a harmonic potential, the ion is illuminated with a specially shaped, 1.5 ns pulse that imparts a momentum kick on the ion with a spin-dependent direction. A fast Pockels cell allows us to change the direction of the spin-dependent kick from each subsequent pulse out of an 80 MHz mode-locked laser. By concatenating a series of these very high fidelity spin-dependent kicks, we separate the ion's wave packet into two, spatially distinct states separated by about 200 recoil momenta and involving about 70 phonons. This method for creating a Schrodinger cat state is not time-limited by the trap frequency, and does not rely on confinement in the Lamb-Dicke regime. This work is supported by grants from the U.S. Army Research Office with funding from the DARPA OLE program, IARPA, and the MURI program; and the NSF Physics Frontier Center at JQI.

Ultrafast magnetization switching by spin-orbit torques

DOE Office of Scientific and Technical Information (OSTI.GOV)

Garello, Kevin, E-mail: kevin.garello@mat.ethz.ch; Avci, Can Onur; Baumgartner, Manuel

2014-11-24

Spin-orbit torques induced by spin Hall and interfacial effects in heavy metal/ferromagnetic bilayers allow for a switching geometry based on in-plane current injection. Using this geometry, we demonstrate deterministic magnetization reversal by current pulses ranging from 180 ps to ms in Pt/Co/AlO{sub x} dots with lateral dimensions of 90 nm. We characterize the switching probability and critical current I{sub c} as a function of pulse length, amplitude, and external field. Our data evidence two distinct regimes: a short-time intrinsic regime, where I{sub c} scales linearly with the inverse of the pulse length, and a long-time thermally assisted regime, where I{sub c} variesmore » weakly. Both regimes are consistent with magnetization reversal proceeding by nucleation and fast propagation of domains. We find that I{sub c} is a factor 3–4 smaller compared to a single domain model and that the incubation time is negligibly small, which is a hallmark feature of spin-orbit torques.« less

Hysteresis, nucleation and growth phenomena in spin-crossover solids

NASA Astrophysics Data System (ADS)

Ridier, Karl; Molnár, Gábor; Salmon, Lionel; Nicolazzi, William; Bousseksou, Azzedine

2017-12-01

The observation and the study of first-order phase transitions in cooperative spin-crossover (SCO) solids exhibiting hysteresis behaviours are of particular interest and currently constitute a burgeoning area in the field of bistable molecular materials. The understanding and the control of the transition mechanisms (nucleation and growth processes) and their dynamics within the hysteresis region appear to be a general and appealing problem from a fundamental point of view and for technological applications as well. This review reports on the recent progresses and most important findings made on the spatiotemporal dynamics of the spin transition in SCO solids, particularly through the universal nucleation and growth process. Both thermally induced and light-induced spin transitions are discussed. We open up this review to the central question of the evolution of the transition mechanisms and dynamics in SCO nano-objects, which constitute promising systems to reach ultra-fast switching, and the experimental issues inherent to such studies at the micro- and nanometric scale.

A sub-femtojoule electrical spin-switch based on optically trapped polariton condensates.

PubMed

Dreismann, Alexander; Ohadi, Hamid; Del Valle-Inclan Redondo, Yago; Balili, Ryan; Rubo, Yuri G; Tsintzos, Simeon I; Deligeorgis, George; Hatzopoulos, Zacharias; Savvidis, Pavlos G; Baumberg, Jeremy J

2016-10-01

Practical challenges to extrapolating Moore's law favour alternatives to electrons as information carriers. Two promising candidates are spin-based and all-optical architectures, the former offering lower energy consumption, the latter superior signal transfer down to the level of chip-interconnects. Polaritons-spinor quasi-particles composed of semiconductor excitons and microcavity photons-directly couple exciton spins and photon polarizations, combining the advantages of both approaches. However, their implementation for spintronics has been hindered because polariton spins can be manipulated only optically or by strong magnetic fields. Here we use an external electric field to directly control the spin of a polariton condensate, bias-tuning the emission polarization. The nonlinear spin dynamics offers an alternative route to switching, allowing us to realize an electrical spin-switch exhibiting ultralow switching energies below 0.5 fJ. Our results lay the foundation for development of devices based on the electro-optical control of coherent spin ensembles on a chip.

High speed photography and photonics applications: An underutilized technology

DOE Office of Scientific and Technical Information (OSTI.GOV)

Paisley, D.L.

1996-10-01

Snapshot: Paisley describes the development of high-speed photography including the role of streak cameras, fiber optics, and lasers. Progress in this field has created a powerful tool for viewing such ultrafast processes as hypersonic events and ballistics. {copyright} {ital 1996 Optical Society of America.} [1047-6938-96-10-9939-04

High-Responsivity Graphene–Boron Nitride Photodetector and Autocorrelator in a Silicon Photonic Integrated Circuit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shiue, Ren-Jye; Gao, Yuanda; Wang, Yifei

2015-11-11

Graphene and other two-dimensional (2D) materials have emerged as promising materials for broadband and ultrafast photodetection and optical modulation. These optoelectronic capabilities can augment complementary metal–oxide–semiconductor (CMOS) devices for high-speed and low-power optical interconnects. Here, we demonstrate an on-chip ultrafast photodetector based on a two-dimensional heterostructure consisting of high-quality graphene encapsulated in hexagonal boron nitride. Coupled to the optical mode of a silicon waveguide, this 2D heterostructure-based photodetector exhibits a maximum responsivity of 0.36 A/W and high-speed operation with a 3 dB cutoff at 42 GHz. From photocurrent measurements as a function of the top-gate and source-drain voltages, we concludemore » that the photoresponse is consistent with hot electron mediated effects. At moderate peak powers above 50 mW, we observe a saturating photocurrent consistent with the mechanisms of electron–phonon supercollision cooling. This nonlinear photoresponse enables optical on-chip autocorrelation measurements with picosecond-scale timing resolution and exceptionally low peak powers.« less

Nonequilibrium phase transitions in cuprates observed by ultrafast electron crystallography.

PubMed

Gedik, Nuh; Yang, Ding-Shyue; Logvenov, Gennady; Bozovic, Ivan; Zewail, Ahmed H

2007-04-20

Nonequilibrium phase transitions, which are defined by the formation of macroscopic transient domains, are optically dark and cannot be observed through conventional temperature- or pressure-change studies. We have directly determined the structural dynamics of such a nonequilibrium phase transition in a cuprate superconductor. Ultrafast electron crystallography with the use of a tilted optical geometry technique afforded the necessary atomic-scale spatial and temporal resolutions. The observed transient behavior displays a notable "structural isosbestic" point and a threshold effect for the dependence of c-axis expansion (Deltac) on fluence (F), with Deltac/F = 0.02 angstrom/(millijoule per square centimeter). This threshold for photon doping occurs at approximately 0.12 photons per copper site, which is unexpectedly close to the density (per site) of chemically doped carriers needed to induce superconductivity.

Ultrafast, large-field multiphoton microscopy based on an acousto-optic deflector and a spatial light modulator.

PubMed

Shao, Yonghong; Qin, Wan; Liu, Honghai; Qu, Junle; Peng, Xiang; Niu, Hanben; Gao, Bruce Z

2012-07-01

We present an ultrafast, large-field multiphoton excitation fluorescence microscope with high lateral and axial resolutions based on a two-dimensional (2-D) acousto-optical deflector (AOD) scanner and spatial light modulator (SLM). When a phase-only SLM is used to shape the near-infrared light from a mode-locked titanium:sapphire laser into a multifocus array including the 0-order beam, a 136 μm × 136 μm field of view is achieved with a 60× objective using a 2-D AOD scanner without any mechanical scan element. The two-photon fluorescence image of a neuronal network that was obtained using this system demonstrates that our microscopy permits observation of dynamic biological events in a large field with high-temporal and -spatial resolution.

Confocal Raman imaging of optical waveguides in LiNbO3 fabricated by ultrafast high-repetition rate laser-writing.

PubMed

Ródenas, Airán; Nejadmalayeri, Amir H; Jaque, Daniel; Herman, Peter

2008-09-01

We report on the confocal Raman characterization of the micro-structural lattice changes induced during the high-repetition rate ultrafast laser writing of buried optical waveguides in lithium niobate (LiNbO(3)) crystals. While the laser beam focal volume is characterized by a significant lattice expansion together with a high defect concentration, the adjacent waveguide zone is largely free of defects, undergoing only slight rearrangement of the oxygen octahedron in the LiNbO(3) lattice. The close proximity of these two zones has been found responsible for the propagation losses of the guided light. Subjacent laser-induced periodic micro-structures have been also observed inside the laser focal volume, and identified with a strong periodic distribution of lattice defects.

Modulation of ultrafast laser-induced magnetization precession in BiFeO3-coated La0.67Sr0.33MnO3 thin films

NASA Astrophysics Data System (ADS)

Wan, Qian; Jin, KuiJuan; Wang, JieSu; Yao, HongBao; Gu, JunXing; Guo, HaiZhong; Xu, XiuLai; Yang, GuoZhen

2017-04-01

The ultrafast laser-excited magnetization dynamics of ferromagnetic (FM) La0.67Sr0.33MnO3 (LSMO) thin films with BiFeO3 (BFO) coating layers grown by laser molecular beam epitaxy are investigated using the optical pump-probe technique. Uniform magnetization precessions are observed in the films under an applied external magnetic field by measuring the time-resolved magneto-optical Kerr effect. The magnetization precession frequencies of the LSMO thin films with the BFO coating layers are lower than those of uncoated LSMO films, which is attributed to the suppression of the anisotropy field induced by the exchange interaction at the interface between the antiferromagnetic order of BFO and the FM order of LSMO.

Ultrafast dynamics and stabilization in chip-scale optical frequency combs (Conference Presentation)

NASA Astrophysics Data System (ADS)

Huang, Shu Wei

2017-02-01

Optical frequency comb technology has been the cornerstone for scientific breakthroughs such as precision frequency metrology, re-definition of time, extreme light-matter interaction, and attosecond sciences. Recently emerged Kerr-active microresonators are promising alternatives to the current benchmark femtosecond laser platform. These chip-scale frequency combs, or Kerr combs, are unique in their compact footprints and offer the potential for monolithic electronic and feedback integration, thereby expanding the already remarkable applications of optical frequency combs. In this talk, I will first report the generation and characterization of low-phase-noise Kerr frequency combs. Measurements of the Kerr comb ultrafast dynamics and phase noise will be presented and discussed. Then I will describe novel strategies to fully stabilize Kerr comb line frequencies towards chip-scale optical frequency synthesizers with a relative uncertainty better than 2.7×10-16. I will show that the unique generation physics of Kerr frequency comb can provide an intrinsic self-referenced access to the Kerr comb line frequencies. The strategy improves the optical frequency stability by more than two orders of magnitude, while preserving the Kerr comb's key advantage of low SWaP and potential for chip-scale electronic and photonic integration.

Semimetallization of dielectrics in strong optical fields

PubMed Central

Kwon, Ojoon; Paasch-Colberg, Tim; Apalkov, Vadym; Kim, Bum-Kyu; Kim, Ju-Jin; Stockman, Mark I.; Kim, D.

2016-01-01

At the heart of ever growing demands for faster signal processing is ultrafast charge transport and control by electromagnetic fields in semiconductors. Intense optical fields have opened fascinating avenues for new phenomena and applications in solids. Because the period of optical fields is on the order of a femtosecond, the current switching and its control by an optical field may pave a way to petahertz optoelectronic devices. Lately, a reversible semimetallization in fused silica on a femtosecond time scale by using a few-cycle strong field (~1 V/Å) is manifested. The strong Wannier-Stark localization and Zener-type tunneling were expected to drive this ultrafast semimetallization. Wider spread of this technology demands better understanding of whether the strong field behavior is universally similar for different dielectrics. Here we employ a carrier-envelope-phase stabilized, few-cycle strong optical field to drive the semimetallization in sapphire, calcium fluoride and quartz and to compare this phenomenon and show its remarkable similarity between them. The similarity in response of these materials, despite the distinguishable differences in their physical properties, suggests the universality of the physical picture explained by the localization of Wannier-Stark states. Our results may blaze a trail to PHz-rate optoelectronics. PMID:26888147

Semimetallization of dielectrics in strong optical fields

DOE PAGES

Kwon, Ojoon; Paasch-Colberg, Tim; Apalkov, Vadym; ...

2016-02-18

At the heart of ever growing demands for faster signal processing is ultrafast charge transport and control by electromagnetic fields in semiconductors. Intense optical fields have opened fascinating avenues for new phenomena and applications in solids. Because the period of optical fields is on the order of a femtosecond, the current switching and its control by an optical field may pave a way to petahertz optoelectronic devices. Lately, a reversible semimetallization in fused silica on a femtosecond time scale by using a few-cycle strong field (~1 V/Å) is manifested. The strong Wannier-Stark localization and Zener-type tunneling were expected to drivemore » this ultrafast semimetallization. Wider spread of this technology demands better understanding of whether the strong field behavior is universally similar for different dielectrics. Here we employ a carrier-envelope-phase stabilized, few-cycle strong optical field to drive the semimetallization in sapphire, calcium fluoride and quartz and to compare this phenomenon and show its remarkable similarity between them. The similarity in response of these materials, despite the distinguishable differences in their physical properties, suggests the universality of the physical picture explained by the localization of Wannier-Stark states. Lastly, our results may blaze a trail to PHz-rate optoelectronics.« less

The effect of excitation intensity variation and silver nanoparticle codoping on nonlinear optical properties of mixed tellurite and zinc oxide glass doped with Nd2O3 studied through ultrafast z-scan spectroscopy

NASA Astrophysics Data System (ADS)

Moreira, L.; Falci, R. F.; Darabian, H.; Anjos, V.; Bell, M. J. V.; Kassab, L. R. P.; Bordon, C. D. S.; Doualan, J. L.; Camy, P.; Moncorgé, R.

2018-05-01

The research on Nd3+ doped new solid-state laser hosts with specific thermo-mechanical and optical properties is very active. Nd3+ doped tellurite glasses are suitable for these applications. They have high linear and nonlinear refraction index, wide transmittance range. The TeO2-ZnO (TZO) glass considered in the present work combines all those features and the nonlinear optical properties can be used for the development of Kerr-lens mode-locked sub picosecond lasers. Recently the laser performance of Nd3+ doped TZO glass and was reported and laser slope efficiency of 21% was observed. We investigate how the intensity variation and the silver nanoparticles codoping affects the nonlinear optical properties of Nd3+ doped TZO glasses. Intensity dependent nonlinear refraction indices coefficients at 750, 800 and 850 nm were observed. The nonlinear optical features were obtained through ultrafast single beam z-scan technique with excitations at 750, 800 and 850 nm and are up to two orders of magnitude higher than those reported in the literature.

Semimetallization of dielectrics in strong optical fields.

PubMed

Kwon, Ojoon; Paasch-Colberg, Tim; Apalkov, Vadym; Kim, Bum-Kyu; Kim, Ju-Jin; Stockman, Mark I; Kim, D

2016-02-18

At the heart of ever growing demands for faster signal processing is ultrafast charge transport and control by electromagnetic fields in semiconductors. Intense optical fields have opened fascinating avenues for new phenomena and applications in solids. Because the period of optical fields is on the order of a femtosecond, the current switching and its control by an optical field may pave a way to petahertz optoelectronic devices. Lately, a reversible semimetallization in fused silica on a femtosecond time scale by using a few-cycle strong field (~1 V/Å) is manifested. The strong Wannier-Stark localization and Zener-type tunneling were expected to drive this ultrafast semimetallization. Wider spread of this technology demands better understanding of whether the strong field behavior is universally similar for different dielectrics. Here we employ a carrier-envelope-phase stabilized, few-cycle strong optical field to drive the semimetallization in sapphire, calcium fluoride and quartz and to compare this phenomenon and show its remarkable similarity between them. The similarity in response of these materials, despite the distinguishable differences in their physical properties, suggests the universality of the physical picture explained by the localization of Wannier-Stark states. Our results may blaze a trail to PHz-rate optoelectronics.

Attosecond electron pulse trains and quantum state reconstruction in ultrafast transmission electron microscopy

NASA Astrophysics Data System (ADS)

Priebe, Katharina E.; Rathje, Christopher; Yalunin, Sergey V.; Hohage, Thorsten; Feist, Armin; Schäfer, Sascha; Ropers, Claus

2017-12-01

Ultrafast electron and X-ray imaging and spectroscopy are the basis for an ongoing revolution in the understanding of dynamical atomic-scale processes in matter. The underlying technology relies heavily on laser science for the generation and characterization of ever shorter pulses. Recent findings suggest that ultrafast electron microscopy with attosecond-structured wavefunctions may be feasible. However, such future technologies call for means to both prepare and fully analyse the corresponding free-electron quantum states. Here, we introduce a framework for the preparation, coherent manipulation and characterization of free-electron quantum states, experimentally demonstrating attosecond electron pulse trains. Phase-locked optical fields coherently control the electron wavefunction along the beam direction. We establish a new variant of quantum state tomography—`SQUIRRELS'—for free-electron ensembles. The ability to tailor and quantitatively map electron quantum states will promote the nanoscale study of electron-matter entanglement and new forms of ultrafast electron microscopy down to the attosecond regime.

Large lateral photovoltaic effect with ultrafast relaxation time in SnSe/Si junction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Xianjie; Zhao, Xiaofeng; Hu, Chang

In this paper, we report a large lateral photovoltaic effect (LPE) with ultrafast relaxation time in SnSe/p-Si junctions. The LPE shows a linear dependence on the position of the laser spot, and the position sensitivity is as high as 250 mV mm{sup −1}. The optical response time and the relaxation time of the LPE are about 100 ns and 2 μs, respectively. The current-voltage curve on the surface of the SnSe film indicates the formation of an inversion layer at the SnSe/p-Si interface. Our results clearly suggest that most of the excited-electrons diffuse laterally in the inversion layer at the SnSe/p-Si interface, whichmore » results in a large LPE with ultrafast relaxation time. The high positional sensitivity and ultrafast relaxation time of the LPE make the SnSe/p-Si junction a promising candidate for a wide range of optoelectronic applications.« less

Theory of Direct Optical Measurement of Pure Spin Currents in Direct-gap Semiconductors

NASA Astrophysics Data System (ADS)

Wang, Jing; Liu, Ren-Bao; Zhu, Bang-Fen

2010-01-01

We predict that a pure spin current in a semiconductor may lead to the optical circular birefingence effect without invoking magnetization. This effect may be exploited for a direct, non-destructive measurement of the pure spin current. We derive the effective coupling between a pure spin current and a polarized light beam, and point out that it originates from the inherent spin-orbit coupling in the valence bands, rather than the Rashba or Dresselhaus effects due to inversion asymmetries. The Faraday rotation angle in GaAs is estimated, which indicates that this spin current optical birefringence is experimentally observable.

Strain-assisted optomechanical coupling of polariton condensate spin to a micromechanical resonator

NASA Astrophysics Data System (ADS)

Be'er, O.; Ohadi, H.; del Valle-Inclan Redondo, Y.; Ramsay, A. J.; Tsintzos, S. I.; Hatzopoulos, Z.; Savvidis, P. G.; Baumberg, J. J.

2017-12-01

We report spin and intensity coupling of an exciton-polariton condensate to the mechanical vibrations of a circular membrane microcavity. We optically drive the microcavity resonator at the lowest mechanical resonance frequency while creating an optically trapped spin-polarized polariton condensate in different locations on the microcavity and observe spin and intensity oscillations of the condensate at the vibration frequency of the resonator. Spin oscillations are induced by vibrational strain driving, whilst the modulation of the optical trap due to the displacement of the membrane causes intensity oscillations in the condensate emission. Our results demonstrate spin-phonon coupling in a macroscopically coherent condensate.

Origin of the Ultrafast Response of the Lateral Photovoltaic Effect in Amorphous MoS2/Si Junctions.

PubMed

Hu, Chang; Wang, Xianjie; Miao, Peng; Zhang, Lingli; Song, Bingqian; Liu, Weilong; Lv, Zhe; Zhang, Yu; Sui, Yu; Tang, Jinke; Yang, Yanqiang; Song, Bo; Xu, Ping

2017-05-31

The lateral photovoltaic (LPV) effect has attracted much attention for a long time because of its application in position-sensitive detectors (PSD). Here, we report the ultrafast response of the LPV in amorphous MoS 2 /Si (a-MoS 2 /Si) junctions prepared by the pulsed laser deposition (PLD) technique. Different orientations of the built-in field and the breakover voltages are observed for a-MoS 2 films deposited on p- and n-type Si wafers, resulting in the induction of positive and negative voltages in the a-MoS 2 /n-Si and a-MoS 2 /p-Si junctions upon laser illumination, respectively. The dependence of the LPV on the position of the illumination shows very high sensitivity (183 mV mm -1 ) and good linearity. The optical relaxation time of LPV with a positive voltage was about 5.8 μs in a-MoS 2 /n-Si junction, whereas the optical relaxation time of LPV with a negative voltage was about 2.1 μs in a-MoS 2 /p-Si junction. Our results clearly suggested that the inversion layer at the a-MoS 2 /Si interface made a good contribution to the ultrafast response of the LPV in a-MoS 2 /Si junctions. The large positional sensitivity and ultrafast relaxation of LPV may promise the a-MoS 2 /Si junction's applications in fast position-sensitive detectors.

Ultrafast terahertz electrodynamics of photonic and electronic nanostructures

DOE Office of Scientific and Technical Information (OSTI.GOV)

Luo, Liang

This thesis summarizes my work on using ultrafast laser pulses to study Terahertz (THz) electrodynamics of photonic and electronic nanostructures and microstructures. Ultrafast timeresolved (optical, NIR, MIR, THz) pump-probe spectroscopy setup has been successfully built, which enables me to perform a series of relevant experiments. Firstly, a novel high e ciency and compact THz wave emitter based on split-ring-resonators has been developed and characterized. The emitter can be pumped at any wavelength by tailoring the magnetic resonance and could generate gapless THz waves covering the entire THz band. Secondly, two kinds of new photonic structures for THz wave manipulation havemore » been successfully designed and characterized. One is based on the 1D and 2D photo-imprinted di ractive elements. The other is based on the photoexcited double-split-ring-resonator metamaterials. Both structures are exible and can modulate THz waves with large tunability. Thirdly, the dark excitons in semiconducting singlewalled carbon nanotubes are studied by optical pump and THz probe spectroscopy, which provides the rst insights into the THz responses of nonequilibrium excitonic correlations and dynamics from the dark ground states in carbon nanotubes. Next, several on-going projects are brie y presented such as the study of ultrafast THz dynamics of Dirac fermions in topological insulator Bi 2Se 3 with Mid-infrared excitation. Finally, the thesis ends with a summary of the completed experiments and an outlook of the future plan.« less

Quantitative ultra-fast MRI of HPMC swelling and dissolution.

PubMed

Chen, Ya Ying; Hughes, L P; Gladden, L F; Mantle, M D

2010-08-01

For the first time quantitative Rapid Acquisition with Relaxation Enhancement (RARE) based ultra-fast two-dimensional magnetic resonance imaging has been used to follow the dissolution of hydroxypropylmethyl cellulose (HPMC) in water. Quantitative maps of absolute water concentration, spin-spin relaxation times and water self-diffusion coefficient are obtained at a spatial resolution of 469 microm in less than 3 min each. These maps allow the dynamic development of the medium release rate HPMC/water system to be followed. It is demonstrated that the evolution of the gel layer and, in particular, the gradient in water concentration across it, is significantly different when comparing the quantitative RARE sequence with a standard (nonquantitative) implementation of RARE. The total gel thickness in the axial direction grows faster than that in the radial direction and that the dry core initially expands anisotropically. Additionally, while HPMC absorbs a large amount of water during the dissolution process, the concentration gradient of water within the gel layer is relatively small. For the first time MRI evidence is presented for a transition swollen glassy layer which resides between the outer edge of the dry tablet core and the inner edge of the gel layer. (c) 2010 Wiley-Liss, Inc. and the American Pharmacists Association

Signatures of spin-orbital states of t2g 2 system in optical conductivity: R VO3 (R =Y and La)

NASA Astrophysics Data System (ADS)

Kim, Minjae

2018-04-01

We investigate signatures of the spin and orbital states of R VO3 (R =Y and La) in optical conductivity using density functional theory plus dynamical mean-field theory (DFT+DMFT). From the assignment of multiplet state configurations to optical transitions, the DFT+DMFT reproduces experimental temperature-dependent evolutions of optical conductivity for both YVO3 and LaVO3. We also show that the optical conductivity is a useful quantity to probe the evolution of the orbital state even in the absence of spin order. The result provides a reference to investigate the spin and orbital states of t2g 2 vanadate systems, which is an important issue for both fundamental physics on spin and orbital states and applications of vanadates by means of orbital state control.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhai, Yaxin; Baniya, Sangita; Zhang, Chuang

Two-dimensional (2D) layered hybrid organic-inorganic halide perovskite semiconductors form natural “multiple quantum wells” that have strong spin-orbit coupling due to the heavy elements in their building blocks. This may lead to “Rashba splitting” close to the extrema in the electron bands. We have used a plethora of ultrafast transient, nonlinear optical spectroscopies and theoretical calculations to study the primary (excitons) and long-lived (free carriers) photoexcitations in thin films of 2D perovskite, namely, (C 6H 5C 2H 4NH 3) 2PbI 4. The density functional theory calculation shows the occurrence of Rashba splitting in the plane perpendicular to the 2D barrier. Frommore » the electroabsorption spectrum and photoinduced absorption spectra from excitons and free carriers, we obtain a giant Rashba splitting in this compound, with energy splitting of (40 ± 5) meV and Rashba parameter of (1.6 ± 0.1) eV·Å, which are among the highest Rashba splitting size parameters reported so far. In conclusion, this finding shows that 2D hybrid perovskites have great promise for potential applications in spintronics.« less

Femtosecond direct space-to-time pulse shaping in an integrated-optic configuration.

PubMed

Leaird, D E; Weiner, A M

2004-07-01

We demonstrate femtosecond operation of an integrated-optic direct space-to-time pulse shaper for which there is a direct mapping (no Fourier transform) between the spatial position of the masking function and the temporal position in the output waveform. The apparatus is used to generate trains of more than 30 pulses as an ultrafast optical data packet over approximately an 80-ps temporal window.

Theoretical ultra-fast spectroscopy in transition metal dichalcogenides

NASA Astrophysics Data System (ADS)

Molina-Sanchez, Alejandro; Sangalli, Davide; Marini, Andrea; Wirtz, Ludger

Semiconducting 2D-materials like the transition metal dichalcogenides (TMDs) MoS2, MoSe2, WS2, WSe2 are promising alternatives to graphene for designing novel opto-electronic devices. The strong spin-orbit interaction along with the breaking of inversion symmetry in single-layer TMDs allow using the valley-index as a new quantum number. The practical use of valley physics depends on the lifetimes of valley-polarized excitons which are affected by scattering at phonons, impurities and by carrier-carrier interactions. The carrier dynamics can be monitored using ultra-fast spectroscopies such as pump-probe experiments. The carrier dynamics is simulated using non-equilibrium Green's function theory in an ab-initio framework. We include carrier relaxation through electron-phonon interaction. We obtain the transient absorption spectra of single-layer TMD and compare our simulations with recent pump-probe experiments

Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [ Co ( terpy ) 2 ] 2 +

DOE PAGES

Biasin, Elisa; van Driel, Tim Brandt; Kjær, Kasper S.; ...

2016-06-30

Here, we study the structural dynamics of photoexcited [Co(terpy) 2] 2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of themore » high spin state is established on a single-picosecond time scale and that this state has a lifetime of ~7 ps.« less

Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom

NASA Astrophysics Data System (ADS)

Brauße, Felix; Goldsztejn, Gildas; Amini, Kasra; Boll, Rebecca; Bari, Sadia; Bomme, Cédric; Brouard, Mark; Burt, Michael; de Miranda, Barbara Cunha; Düsterer, Stefan; Erk, Benjamin; Géléoc, Marie; Geneaux, Romain; Gentleman, Alexander S.; Guillemin, Renaud; Ismail, Iyas; Johnsson, Per; Journel, Loïc; Kierspel, Thomas; Köckert, Hansjochen; Küpper, Jochen; Lablanquie, Pascal; Lahl, Jan; Lee, Jason W. L.; Mackenzie, Stuart R.; Maclot, Sylvain; Manschwetus, Bastian; Mereshchenko, Andrey S.; Mullins, Terence; Olshin, Pavel K.; Palaudoux, Jérôme; Patchkovskii, Serguei; Penent, Francis; Piancastelli, Maria Novella; Rompotis, Dimitrios; Ruchon, Thierry; Rudenko, Artem; Savelyev, Evgeny; Schirmel, Nora; Techert, Simone; Travnikova, Oksana; Trippel, Sebastian; Underwood, Jonathan G.; Vallance, Claire; Wiese, Joss; Simon, Marc; Holland, David M. P.; Marchenko, Tatiana; Rouzée, Arnaud; Rolles, Daniel

2018-04-01

Due to its element and site specificity, inner-shell photoelectron spectroscopy is a widely used technique to probe the chemical structure of matter. Here, we show that time-resolved inner-shell photoelectron spectroscopy can be employed to observe ultrafast chemical reactions and the electronic response to the nuclear motion with high sensitivity. The ultraviolet dissociation of iodomethane (CH3I ) is investigated by ionization above the iodine 4 d edge, using time-resolved inner-shell photoelectron and photoion spectroscopy. The dynamics observed in the photoelectron spectra appear earlier and are faster than those seen in the iodine fragments. The experimental results are interpreted using crystal-field and spin-orbit configuration interaction calculations, and demonstrate that time-resolved inner-shell photoelectron spectroscopy is a powerful tool to directly track ultrafast structural and electronic transformations in gas-phase molecules.

Black phosphorus quantum dots for femtosecond laser photonics

NASA Astrophysics Data System (ADS)

Liu, Meng; Jiang, Xiao-Fang; Yan, Yu-Rong; Wang, Xu-De; Luo, Ai-Ping; Xu, Wen-Cheng; Luo, Zhi-Chao

2018-01-01

As a rising two-dimensional (2D) nanomaterial, layered black phosphorus (BP) nanosheets have shown promising applications in electronics and photonics. Besides the 2D layered structure, recently black phosphorus quantum dots (BPQDs) exhibiting unique optoelectronic properties had been successfully fabricated. However, the nonlinear optical properties of BPQDs at the telecommunication band have not been investigated. Herein, we synthesized the BPQDs by using a liquid exfoliation method that combined probe sonication and bath sonication. It was found that the evident saturable absorption ability of BPQDs at 1.55 μm waveband could be clearly observed. As for the applications of ultrafast photonics, we fabricated the BPQDs saturable absorber (BPQDs-SA) and applied it to an ultrafast laser. By virtue of the excellent nonlinear optical properties of BPQDs, the fiber laser delivers the stable pulse train with duration as short as 291 fs, whose performance could, to the best of our knowledge, compete with nowadays' commercial optical saturable absorber devices. In addition, due to the highly nonlinear optical effect generated by the fabricated BPQDs-SA, the multi-soliton nonlinear dynamics in the fiber laser were also investigated. The obtained results suggest that the BPQDs could be an attractive nonlinear optical material for applications in the field of nonlinear optics.

Chemical modulation of electronic structure at the excited state

NASA Astrophysics Data System (ADS)

Li, F.; Song, C.; Gu, Y. D.; Saleem, M. S.; Pan, F.

2017-12-01

Spin-polarized electronic structures are the cornerstone of spintronics, and have thus attracted a significant amount of interest; in particular, researchers are looking into how to modulate the electronic structure to enable multifunctional spintronics applications, especially in half-metallic systems. However, the control of the spin polarization has only been predicted in limited two-dimensional systems with spin-polarized Dirac structures and is difficult to achieve experimentally. Here, we report the modulation of the electronic structure in the light-induced excited state in a typical half-metal, L a1 /2S r1 /2Mn O3 -δ . According to the spin-transport measurements, there appears a light-induced increase in magnetoresistance due to the enhanced spin scattering, which is closely associated with the excited spin polarization. Strikingly, the light-induced variation can be enhanced via alcohol processing and reduced by oxygen annealing. X-ray photoelectron spectroscopy measurements show that in the chemical process, a redox reaction occurs with a change in the valence of Mn. Furthermore, first-principles calculations reveal that the change in the valence of Mn alters the electronic structure and consequently modulates the spin polarization in the excited state. Our findings thus report a chemically tunable electronic structure, demonstrating interesting physics and the potential for multifunctional applications and ultrafast spintronics.

Optical pumping of the electronic and nuclear spin of single charge-tunable quantum dots.

PubMed

Bracker, A S; Stinaff, E A; Gammon, D; Ware, M E; Tischler, J G; Shabaev, A; Efros, Al L; Park, D; Gershoni, D; Korenev, V L; Merkulov, I A

2005-02-04

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.

Optical Pumping of the Electronic and Nuclear Spin of Single Charge-Tunable Quantum Dots

NASA Astrophysics Data System (ADS)

Bracker, A. S.; Stinaff, E. A.; Gammon, D.; Ware, M. E.; Tischler, J. G.; Shabaev, A.; Efros, Al. L.; Park, D.; Gershoni, D.; Korenev, V. L.; Merkulov, I. A.

2005-02-01

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the net charge from positive to neutral to negative with a charge-tunable heterostructure. Negative photoluminescence polarization memory is enhanced by optical pumping of ground state electron spins, which we prove with the first measurements of the Hanle effect on an individual quantum dot. We use the Overhauser effect in a high longitudinal magnetic field to demonstrate efficient optical pumping of nuclear spins for all three charge states of the quantum dot.

Ultrafast FADC multiplexer

NASA Astrophysics Data System (ADS)

Mirzoyan, R.; Cortina, J.; Lorenz, E.; Martinez, M.; Ostankov, A.; Paneque, D.

2002-10-01

Ultrafast Flash amplitude-to-digital converters (FADCs) are still very expensive. Here we propose a multiplexing scheme allowing one in common trigger mode to read out multiple signal sources by using a single FADC channel. Usual coaxial cables can be used in the multiplexer as analog signal delay elements. The limited bandwidth of the coaxial cable, depending on its type and length will set an upper limit to the number of multiplexed channels. Better bandwidth and the correspondingly higher number of multiplexed channels one can obtain when using the technique of transmission of analog signals via optical fibers. Low-cost vertical cavity surface emitting laser (VCSEL) diodes can be used as converters of fast electrical signals into near infrared light. Multiplexing can be an economically priced solution when one needs ultrafast digitization of hundreds of fast signal channels.

Coherent helix vacancy phonon and its ultrafast dynamics waning in topological Dirac semimetal C d3A s2

NASA Astrophysics Data System (ADS)

Sun, Fei; Wu, Q.; Wu, Y. L.; Zhao, H.; Yi, C. J.; Tian, Y. C.; Liu, H. W.; Shi, Y. G.; Ding, H.; Dai, X.; Richard, P.; Zhao, Jimin

2017-06-01

We report an ultrafast lattice dynamics investigation of the topological Dirac semimetal C d3A s2 . A coherent phonon beating among three evenly spaced A1 g optical phonon modes (of frequencies 1.80, 1.96, and 2.11 THz, respectively) is unambiguously observed. The two side modes originate from the counter helixes composing Cd vacancies. Significantly, such helix vacancy-induced phonon (HVP) modes experience prominent extra waning in their ultrafast dynamics as temperature increases, which is immune to the central mode. Above 200 K, the HVP becomes inactive, which may potentially affect the topological properties. Our results in the lattice degree of freedom suggest the indispensable role of temperature in considering topological properties of such quantum materials.

Ultrafast Pulse Generation in an Organic Nanoparticle-Array Laser.

PubMed

Daskalakis, Konstantinos S; Väkeväinen, Aaro I; Martikainen, Jani-Petri; Hakala, Tommi K; Törmä, Päivi

2018-04-11

Nanoscale coherent light sources offer potentially ultrafast modulation speeds, which could be utilized for novel sensors and optical switches. Plasmonic periodic structures combined with organic gain materials have emerged as promising candidates for such nanolasers. Their plasmonic component provides high intensity and ultrafast nanoscale-confined electric fields, while organic gain materials offer fabrication flexibility and a low acquisition cost. Despite reports on lasing in plasmonic arrays, lasing dynamics in these structures have not been experimentally studied yet. Here we demonstrate, for the first time, an organic dye nanoparticle-array laser with more than a 100 GHz modulation bandwidth. We show that the lasing modulation speed can be tuned by the array parameters. Accelerated dynamics is observed for plasmonic lasing modes at the blue side of the dye emission.

Ultrafast active control of UV light with plasmonic resonance on aluminum nanostripes

NASA Astrophysics Data System (ADS)

Wang, Kuidong; Li, Runze; Hsiao, Hui-Hsin; Chen, Long; Zhang, Haijuan; Chen, Jie

2018-05-01

Ultrafast active control of UV light with aluminum may become an efficient way for high-speed active UV devices. However, the nonlinear optical response of aluminum in the UV region is extremely small, which impedes the realization of the promising modulation depth on ultrafast control. Here, by using the surface plasmon resonance effect, we have achieved a 55-times enhancement in the modulation depth, as well as a short switching time of several picoseconds. Further investigation showed that such an enhancement mainly resulted from a two-order-of-magnitude boost in the response of the signal light to the lattice thermal variation at the plasmonic resonance condition. This improvement in the probing sensitivity could serve as an effective approach to resolve the dynamics of lattice vibrations in metals.

Development of a high brightness ultrafast Transmission Electron Microscope based on a laser-driven cold field emission source.

PubMed

Houdellier, F; Caruso, G M; Weber, S; Kociak, M; Arbouet, A

2018-03-01

We report on the development of an ultrafast Transmission Electron Microscope based on a cold field emission source which can operate in either DC or ultrafast mode. Electron emission from a tungsten nanotip is triggered by femtosecond laser pulses which are tightly focused by optical components integrated inside a cold field emission source close to the cathode. The properties of the electron probe (brightness, angular current density, stability) are quantitatively determined. The measured brightness is the largest reported so far for UTEMs. Examples of imaging, diffraction and spectroscopy using ultrashort electron pulses are given. Finally, the potential of this instrument is illustrated by performing electron holography in the off-axis configuration using ultrashort electron pulses. Copyright © 2017 Elsevier B.V. All rights reserved.

Spin microscope based on optically detected magnetic resonance

DOEpatents

Berman, Gennady P [Los Alamos, NM; Chernobrod, Boris M [Los Alamos, NM

2010-06-29

The invention relates to scanning magnetic microscope which has a photoluminescent nanoprobe implanted in the tip apex of an atomic force microscope (AFM), a scanning tunneling microscope (STM) or a near-field scanning optical microscope (NSOM) and exhibits optically detected magnetic resonance (ODMR) in the vicinity of unpaired electron spins or nuclear magnetic moments in the sample material. The described spin microscope has demonstrated nanoscale lateral resolution and single spin sensitivity for the AFM and STM embodiments.

Spin microscope based on optically detected magnetic resonance

DOEpatents

Berman, Gennady P.; Chernobrod, Boris M.

2009-11-10

The invention relates to scanning magnetic microscope which has a photoluminescent nanoprobe implanted in the tip apex of an atomic force microscope (AFM), a scanning tunneling microscope (STM) or a near-field scanning optical microscope (NSOM) and exhibits optically detected magnetic resonance (ODMR) in the vicinity of impaired electron spins or nuclear magnetic moments in the sample material. The described spin microscope has demonstrated nanoscale lateral resolution and single spin sensitivity for the AFM and STM embodiments.